Unveiling the Synergistic Effects in Graphene-Based Composites as a New Strategy for High Performance and Sustainable Material Development: A Critical Review

Xiao, Jie; Gao, Xingxing; Xu, Jie; Tan, Juzhong; Zhang, Xuesong; Zhang, Hongchao

doi:10.3390/su172210058

Open AccessReview

Unveiling the Synergistic Effects in Graphene-Based Composites as a New Strategy for High Performance and Sustainable Material Development: A Critical Review

by

Jie Xiao

^1,†,

Xingxing Gao

^1,†,

Jie Xu

^2,*,

Juzhong Tan

³,

Xuesong Zhang

⁴ and

Hongchao Zhang

^1,*

¹

Key Laboratory of Fruit and Vegetable Processing of Ministry of Agriculture and Rural Affairs, Beijing Key Laboratory for Food Non-Thermal Processing, College of Food Science and Nutritional Engineering, China Agriculture University, Beijing 100083, China

²

Center for Nanotechnology and Nanotoxicology, Department of Environmental Health, Harvard T. H. Chan School of Public Health, Harvard University, Boston, MA 02115, USA

³

Department of Animal and Food Sciences, University of Delaware, Newark, DE 19716, USA

⁴

Engineering Laboratory for AgroBiomass Recycling & Valorizing, College of Engineering, China Agricultural University, Beijing 100083, China

^*

Authors to whom correspondence should be addressed.

^†

These authors contributed equally to this work.

Sustainability 2025, 17(22), 10058; https://doi.org/10.3390/su172210058

Submission received: 28 August 2025 / Revised: 26 October 2025 / Accepted: 5 November 2025 / Published: 11 November 2025

(This article belongs to the Section Sustainable Materials)

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Abstract

Graphene-based materials have been the subject of extensive scientific investigations owing to their distinctive properties and versatile functionalities. However, their applications are hindered due to limited material performance, difficulties in recycling, and high costs during manufacturing. Considering this, studies have developed graphene or its derivatives by combining it with other components, while some of these composites revealed significantly improved performance with lesser consumption of raw materials; the underlying mechanisms remain inadequately elucidated. Therefore, the aspiration for novel applications of graphene-based materials could be significantly improved with the full utilization of the synergistic effects of these materials. In this review, we intend to discuss the synergistic activities and their inherent mechanisms between graphene or its derivatives and metals, metal oxides, polymers, and bioactive compounds, among others. The effectiveness of synergisms in enhancing the performance of graphene-based composites is corroborated by studies in a variety of application areas such as antimicrobial materials, cancer therapy, sensors, electronic devices, catalysts, and more. The content presented will be useful to guide the future development of graphene-based materials that are highly efficient and environmentally friendly.

Keywords:

graphene; nanocomposite; diverse applications; synergistic effects; mechanisms; photothermal; electrocatalysis

1. Introduction

Graphene, a two-dimensional (2D) honeycomb lattice of sp²-bonded carbon atoms, and its derivatives (e.g., graphene oxide (GO), reduced GO (rGO), and functionalized variants) have emerged as quintessential model systems for probing interfacial phenomena in materials science [1]. Synthesized via oxidative exfoliation of graphite, GO exemplifies interfacial modification through covalent grafting of oxygen-containing functional groups (epoxy, carbonyl, carboxyl) onto its basal planes and edges, creating reactive sites for subsequent conjugation with polymers, metals, or biomolecules—a cornerstone of composite design [2,3,4]. Conversely, the reduction of GO to rGO partially restores the sp²-conjugated network, dynamically tuning electronic properties and wettability, thereby offering a versatile toolkit for tailoring interactions in hybrid systems [5]. Although pristine graphene derivatives possess exceptional intrinsic properties—such as an ultra-high specific surface area (2630 m²·g⁻¹) and outstanding mechanical strength—their widespread commercialization remains constrained by several critical challenges. These include the high cost of scalable production of high-quality materials, difficulties in processing and integration into existing manufacturing systems, and the complex, often unpredictable relationship between their structural characteristics (e.g., number of layers, defect density) and the resulting performance in specific applications. For instance, irreversible aggregation due to van der Waals forces and π-π stacking compromises accessible surface areas, while inadequate adhesion in standalone graphene sheets restricts charge/energy transfer efficiency in applications like catalysis or antimicrobial surfaces [6,7,8]. Such limitations underscore the necessity of engineering strategies to harness graphene’s full potential.

Recent advances in graphene-based composites emphasize the deliberate integration of graphene with secondary components (metals, metal oxides, polymers) through interfacial bonding mechanisms—covalent coupling, π-π interactions, or electrostatic adsorption [9,10]. The exceptional performance of graphene-based composites originates from the intrinsic properties of graphene and its derivatives, possibly improved with the contributions from additive components to form composites. The essential properties of graphene-based composites include extremely high specific surface area, exceptional mechanical properties, outstanding electrical conductivity, and excellent thermal properties, among others [5,11]. For example, in antimicrobial systems, graphene–metal oxide hybrids leverage both the physical disruption of bacterial membranes (via graphene’s sharp edges) and interfacial electron transfer to metal centers for reactive oxygen species (ROS) generation. Similarly, in catalytic applications, the graphene support interface facilitates charge redistribution, optimizing adsorption energies of reactants and intermediates [12,13,14,15]. Such significantly enhanced functionalities may often be referred to as “synergistic effects”, a concept widely recognized in biological systems, which plays an equally pivotal role in materials science [16,17,18,19,20]. Strong synergism not only improves the material’s performance but also significantly reduces the usage of each individual material component while achieving the same target performance, which promotes sustainability in material manufacturing. Despite these advances, most studies focus on final composite performance rather than deconvoluting synergistic contributions. It is also extremely challenging to validate the interactions between graphene and additives dictating synergy and their quantitative correlations. A few studies have discussed the synergistic actions of graphene-based composites. For instance, studies hypothesized that graphene and its derivatives simultaneously exert physical actions by sharp edges and chemical actions by fast electron transfer at the graphene–additive interfaces [21,22]. Others inferred that graphene provides high surface area and charge mobility, while secondary components contribute specific reactivity or stability components (e.g., metal or metal oxide particles) [23].

Therefore, it is of importance to understand the current status of graphene-based composites with synergistic effects and their corresponding mechanisms to determine its enhanced performance in different applications [24].

Based on the statistical data of graphene-based materials obtained through the Web of Science (date of search: 15 August 2025), the number of publications searched with the keyword “graphene composites” increased rapidly from 2010 to 2024 (Figure 1A). It clearly showed that graphene-based composites have been extensively studied within scientific communities. However, systematic reviews of the existence of synergistic effects within graphene composites and mechanistic studies on synergy remain sparse.

Graphene-based composites possess diverse application domains, including antibacterial agents, antiviral therapeutics, cancer treatment, catalysis, surface coatings, energy storage, electrical conduction, mechanical reinforcement, biosensors, anticorrosion, membrane filtration, etc. [3,5,17]. In this review, we have systematically and comprehensively evaluated most of the above-mentioned applications. Unlike other reviews, a particular emphasis is placed on the synergistic effects exhibited by these materials, as illustrated in (Figure 1B). Furthermore, we aim to elucidate the fundamental synergistic mechanisms and propose standardized criteria to distinguish genuine synergy from coincidental enhancements. Our analysis is intended to inspire the rational design of next-generation composite materials with unprecedented multifunctionality and improved sustainability.

2. Synergistic Effects Observed in Graphene-Based Composites

2.1. Antimicrobial Graphene-Based Composites (AGCs)

Moderate levels of antimicrobial actions of graphene and its derivatives have been observed against a wide scope of microorganisms [2,25,26,27]. In recent years, more efforts have been made to develop more efficient engineered composites, i.e., AGCs for realistic applications [28]. The enhanced antimicrobial actions by AGCs relied on the properties of graphene nanosheets, which can cut, insert, or wrap the target microorganisms as well as interracially support the simultaneous attacks from functional additives on similar or different cellular components of microorganisms. As a result, the dual-action properties impart cumulative or intensified stresses on the microorganisms within a short period, causing cell lysis [29], with significantly reduced additive loading. Synergistic effects in AGCs across various application areas are summarized below.

2.1.1. AGCs Revealing Synergistic Effects for Clinic Application

Bacterial infections on wounded skins or soft tissues present major clinical challenges, especially with the rising threat of multidrug-resistant pathogens due to the overuse of antibiotics [30,31]. In vitro studies have initially demonstrated that most AGCs with synergistic enhanced antimicrobial capabilities serve as proper antibiotic alternatives to control bacterial infections caused by organisms including Escherichia coli (E. coli), Staphylococcus aureus (S. aureus), and Proteus mirabilis (P. mirabilis) [32,33,34,35]. In Figure 2A-1, the results show that the spindle-shaped GO and ZnO composite led to an 80% reduction against E. coli and Salmonella typhimurium (S. typhimurium) compared to only 15% for ZnO or GO alone. However, such trends were not observed for other tested microorganisms. At the same concentration, it exhibited significantly stronger antimicrobial activity, making the composites a promising material for medical application [36]. It has been proposed that GO nanosheets may facilitate the entry of ZnO nanoparticles by disrupting bacterial walls (Figure 2A-2), while the liberated Zn²⁺ could bind to cell membranes and deactivate proteins and enzymes crucial for bacterial growth, chiefly targeting their thiol group (-SH) [36,37]. Thermally reduced graphene oxide (TRGO) combined with ZnO was also reported to exhibit superior bioactivity compared to ZnO and TRGO alone against biofilms of S. aureus, E. coli, and Pseudomonas aeruginosa, which could present in the wound. Beyond functional efficacy, systematic evaluation under wound healing conditions confirmed both biocompatibility and safety, positioning TRGO/ZnO nanocomposites as a new generation of clinically viable bioactive nanomaterials [38].

GO-AgNPs composites, synthesized by complexing Ag and GO, have also shown this synergistic inhibitory effect. GO-AgNPs exhibited a 73% inhibition rate against E. coli and 98.5% against S. aureus. In contrast, GO and AgNPs only displayed an 11% and 18% antibacterial effect, respectively, against E. coli, but this increased to 43% and 52% for S. aureus. This indicates that lower doses of GO-AgNP composites can achieve effective microbial inhibition, attributable to both enhanced bacterial surface adhesion and a higher rate of reactive oxygen species (ROS) production [41]. The inhibitory effects of AGCs on Gram-positive and Gram-negative bacteria are subjected to distinctive behaviors due to the significant variability in the structure of their cell walls. Graphene-based composites are less effective against Gram-negative bacteria, probably owing to their outer membrane composed of a glycerophospholipid and a lipooligosaccharide layer on their surface. The outer membrane protects Gram-negative bacteria from external damage, such as reactive oxygen species [42]. AGCs containing metals or metal oxides are also used as disinfection agents in surface coatings on medical devices to protect material surfaces against microbial adhesion and biofilm formation [43]. Remarkably, the developed rGO-nAg composites, using a simple complexation method, can eradicate nearly 100% S. aureus and P. mirabilis within 2 h–2.5 h, whereas rGO and nAg achieved complete inhibition by the end of 4 h [34]. The physical interaction of the sharp edges of rGO sheets [44,45], along with rGO’s entrapment of bacterial membranes, ensuring higher local silver ion concentrations, contributes to the increase in the permeation of Ag+ into the bacteria [34]. The composite achieved comparable effects within a shorter time frame, indicating that specific metal or metal oxide-based AGCs can exhibit synergistic effects. A deeper understanding of the physical and chemical interactions at the interface between AGCs and bacteria, however, is still necessary.

Antimicrobial hydrogels, known for their optimal water retention properties, have become a focal point for the development of wound dressings. Jian et al. developed an antibacterial hydrogel with controlled water loss by incorporating modified graphene oxide (MGO) into a thermoplastic polyurethane (TPU) matrix. The obtained material (MGO-TPU) inhibited 90.49% of bacteria on mouse tissues, whereas both TPU-GO (61.81% reduction) and TPU-polyhexamethylene guanidine hydrochloride (33.84% reduction) showed limited inhibition rates. Moreover, wounds treated with MGO-TPU healed notably quicker than those treated with other materials (Figure 2B) [39]. The results indicated potential synergies for enhancing wound healing capacity, although the authors did not explicitly state this. Similarly, polydopamine-coated bioactive glass (BGs@PDA) was integrated with reduced graphene oxide (rGO) to enable synergistic antibacterial therapy through silver nanoclusters (AgNCs) and near-infrared (NIR) photothermal activation. In co-culture experiments with both S. aureus and E. coli, the composite achieved nearly 100% bactericidal efficiency [46]. In vivo studies using mouse models have similarly reported wound healing effects with the treatment of Azithromycin @GO-polyethyleneimine-citraconic anhydride [43], GO/quaternary ammonium salt [44], Rose Bengal/GO/Polyvinyl alcohol (PVA) hydrogen [45], or graphene oxide/Ag/Collagen Coating [47].

Additionally, AGCs have displayed enhanced effectiveness in tackling bacterial infections caused by methicillin-resistant Staphylococcus aureus (MRSA) [31,44,48]. This improved effectiveness was observed in curcumin/GO [49] and gallic acid/GO [50]. It was reported that GO can be inserted into the bacterial membrane to deliver the poorly soluble curcumin to fight against MRSA due to its high loading surface area. While GO alone showed no bacterial inhibition at concentrations below 37.5 mg/mL, curcumin/GO showed efficacy against MRSA at a concentration of less than 0.002 mg/mL [49]. The authors indicated a synergistic activity of GO and curcumin based on the minimum inhibitory concentration (MIC) of curcumin in the literature, ranging from 125 mg/mL to 256 mg/mL, whereas no testing of curcumin alone was performed. When irradiated by near-infrared (NIR) light, AGCs quickly absorb optical energy and convert it to localized heat above 50 °C. NIR acts synergistically against microorganisms due to the additional membrane stresses or increased sensitivity of microbes to Au nanostar nanocomposite (AuNS) within the AGCs at elevated temperatures [50,51]. Enhanced by NIR, rGO/AuNS prepared using the seed-mediated growth method exhibited 90% MRSA eradication within 6 min, higher than rGO/AuNS without NIR (less than 16%) and NIR alone (almost none). Graphene sheets facilitated AuNS-mediated disruption of the bacterial cell membrane, increasing direct contact with the cells and, thus, antimicrobial efficacy [48]. The clinical application of metal-based antimicrobial agents may pose potential toxicity risks. There is a necessary need for more research on the biocompatibility and cell toxicity of developed AGCs.

Based on the observed antimicrobial effects and underlying mechanisms of various ACGs, it can be inferred that the unique spatial structure of graphene enables enhanced bacterial membrane adhesion, potentially through physical insertion into the lipid bilayer. This facilitates the delivery of antimicrobial agents. Furthermore, ACGs facilitate the transfer of reactive oxygen species (ROS), which assists in disrupting the bacterial cell membrane and thereby intensifies its antimicrobial efficacy. This multi-faceted mechanism supports its promising potential for clinical applications, such as wound dressings, antibacterial coatings, and targeted antimicrobial therapies. In addition, using AGCs for denture fabrication, restorative treatment, or implant coating in dental treatments has been summarized elsewhere [52].

2.1.2. AGCs Revealing Synergistic Effects for Water Purification

The presence of pathogens in water systems seriously threatens human health [53]. Employing polymer-based AGC films in water purification presents a promising tactic to eliminate pathogenic microorganisms while preserving water quality. The films operate via membrane filtration, where GO physically damages the bacterial membrane due to its high specific area with numerous functional groups, such as hydroxyl, carboxyl, and epoxy groups [54,55]. Assembly of pi-conjugated quaternary ammonium groups (piQA) with hydrothermally formed rGO hydrogel quickly kill most E. coli within 110 s, in contrast to the 10 min inactivation time of piQA alone, and significantly reduced processing time while enhancing antimicrobial efficiency. However, rGO led to a viability reduction of just under 30%. The high antibacterial performance of piQA-rGO may be influenced by the interactions between bacteria and the QA group, as well as the high local concentration of QA groups resulting from the rGO hydrogel’s surface area and porosity [56]. Another promising material, ε-poly-L-lysine (PLL), can be used to covalently functionalize hierarchically porous GO sponge for water treatment. This resulted in 61% retention of E. coli and 53% retention of B. subtilis, which is significantly higher than the 25% and 5% retention rates observed for the GO sponge without PLL, respectively. Moreover, the effective PLL concentration for synthesizing GO/PLL was less than half of the MIC value. The improved bacteria retention is likely due to a synergistic combination of physicochemical attachment and physical straining [57]. The demineralization of synthetic wastewater using AGC materials revealed the low photocatalytic performance of graphene oxide and its reduced form. However, the photothermal conversion efficacy of ZnO-GO [37] and Ni-rGO [58] under NIR irradiation was markedly enhanced compared to the usage of the individual material. The intense localized hyperthermia caused by excellent photocatalytic performance can substantially compromise cell membrane integrity and promote cellular glutathione oxidation, rendering bacteria vulnerable to ROS generated from the separation of photoinduced electrons or holes. Notably, the long-term removal efficacy and stability of AGCs for water purification still require validation to confirm the duration of their synergistic effect, particularly in the format of a film.

2.1.3. AGCs Revealing Synergistic Effects for Packaging Development

Microbial contamination presents a significant threat to food safety, leading to both economic losses and potential health risks. Developing packaging with AGCs is a possible way to decontaminate microorganisms as well as reduce unsustainable material consumption. Graphene sheets combined with food-grade polymers, such as poly (lactic acid) (PLA) and PVA have demonstrated synergistic antimicrobial effects. Additionally, they exhibit higher biocompatibility and better barrier properties when compared to graphene sheets and polymers used alone [59,60]. Starch/rGO, synthesized using a hydrothermal method, effectively functionalized with amylose and accommodates polyiodide to form starch/rGO/polyiodide nanocomposites. The resulting nanocomposite showed inhibition zones of 22.2 ± 2.2 mm and 20.2 ± 0.9 mm against E. coli and S. aureus, respectively, while starch/rGO alone did not exhibit any inhibition [60]. The authors presented the synthetic routes and antibacterial efficacy of the composites. The bactericidal mechanism was speculated but not experimentally validated. In addition, the synergistic effect of rGO, ZnO, and palladium nanoparticles (Pd NPs) demonstrated enhanced catalytic and antibacterial activities against a range of human pathogens, including P. aeruginosa and Klebsiella pneumoniae (K. pneumonia) [61]. Here, rGO sheets increased reactive surface area for Pd NPs and ZnO particles growth, intensifying their bactericidal power by disturbing cell wall permeability and generating several hydroxyl radicals, leading to cell death. Regrettably, comparisons between the antimicrobial capacities of AGCs, the individual components, and the polymers were not conducted in these studies. Moreover, real food systems are very complex, and when AGCs, including graphene and non-graphene components (like polyiodide), come into contact with food components, the production of the intended synergistic antimicrobial effect is not guaranteed [62]. Thus, further research is needed to investigate the antimicrobial capacity of AGCs on food products, as well as their impact on food quality when applied directly.

2.1.4. AGCs Revealing Synergistic Effects on Other Antimicrobial Applications

The potency of AGCs extends to miscellaneous applications, including the critical response to the global threat of COVID-19 which underscores the pressing demand for affordable and scalable antiviral materials. Das Jana et al. developed a PVA-based copper–graphene nanocomposite coating that showed strong antiviral activity (64% reduction) in a solid phase, while graphene or Cu alone showed negligible antiviral activity (Figure 2C-1). Graphene sheets can interact with the lipid bilayer membrane of the influenza virus envelope, clustering multiple viruses together on the graphene, which then positions the viruses in proximity to the Cu₂O nanoparticles. Such nanoparticles could disrupt the HA protein, one of the major surface antigens. As depicted in Figure 2C-2, this nanocomposite is transparent and can be used as a cell phone screen protector. The author expected a wider application of this material on other surfaces, such as face masks, doorknobs, and medical instruments [40]. In addition to inhibiting the growth of viruses, AGCs are also highly effective as fungicides. Mancozeb and Cyproconazol, as broad-spectrum fungicides, physically loaded onto GO, can contribute to synergistic antifungal activity against the plant pathogenic fungus Fusarium graminearum. Mancozeb-GO (2.5–80%) and Cyproconazol-GO (34.62–89.13%) composites showed significantly higher efficacy in controlling the mycelial growth of Fusarium graminearum compared to GO (less than 10%), Mancozeb (9.87–67.4%), or Cyproconazol (28.91–70.04%) alone [63]. A similar synergistic antifungal effect was observed with Pyraclostrobin-GO composites [64], demonstrating their potential as ideal candidates for antibacterial surface coatings and plant fungicides. AGCs’ potent antiviral and antifungal characteristics position them ideally for use in antimicrobial surface coatings in medical facilities, protective equipment like face masks, and plant fungicides. However, further research is necessary to investigate the potential impact of the use of these materials on human health and ecosystems.

As demonstrated in Table 1, the material components of AGCs, their capacities as evidenced by key data, and the categories of working mechanisms reported by selective studies with significant synergistic effects aiming to be applied in antimicrobial area are summarized.

Table 1. Representative studies demonstrating significant synergistic antimicrobial effects in AGCs.

Graphene Materials	Synergistic Components	Target Microorganisms	Synergistic Antimicrobial Capacity	Synergistic Mechanisms	Applications	Reference
rGO	Peptide (Cathelicidin-2)	Escherichia coli (E. coli)	The rGO-peptide complex resulted in 21.8 mm and 16.5 mm inhibition zones compared with 13.3 mm with rGO alone.	Unique surface property	Clinic application	Joshi et al., 2020 [25]
GO	ZnO nanoparticles	E. coli Bacillus subtilis (B. subtilis)	ZnO/GO inactivated >80% of E. coli and 90% of B. subtilis, while it only inactivated 15% of E. coli and 50% of B. subtilis in the same condition with ZnO or GO alone.	Cumulative effect	Clinic application	Zhong et al., 2018 [36]
GO	Polyhexamethylene guanidine hydrochloride (PHMG)/thermoplastic polyurethane (TPU)	E. coli Staphylococcus aureus (S. aureus)	GO-PHMG/TPU inactivated 28.21% of E. coli and 30.88% of S. aureus even after 30 days, while PHMG/TPU inactivated 5.22% and 4.56% and GO/TPU inactivated 71.26% for E. coli and 76.96% for S. aureus.	N/A	Clinic application	Jian et al., 2020 [39]
GO	Quaternary ammonium salts (QAS)	E. coli S. aureus	GO-QAS at 200 μg/mL almost completely killed both E. coli and S. aureus, while GO and QAS caused approximately 87% and 92% cell death for S. aureus and 75% and 88% cell death for E. coli, respectively.	Cumulative effect	Clinic application	Liu et al., 2018 [44]
GO	Curcumin	Methicillin-resistant Staphylococcus aureus (MRSA)	Curcumin/GO showed efficacy against MRSA at a concentration below 0.002 mg/mL, while MIC of GO is 37.5 mg/mL and MIC of curcumin alone against MRSA ranges from 125 to 256 mg/mL.	Unique surface property	Clinic application	Bugli et al., 2018 [48]
rGO	Silver nanoparticles	S. aureus Proteus mirabilis (P. mirabilis)	rGO-nAg killed almost 100% of S. aureus and P. mirabilis within 2–2.5 h compared to 4 h with rGO or nAg alone.	Cumulative effect	Clinic application	Prasad et al., 2017 [33]
GO	AgNPs/polydopamine (PDA)/Ti	E. coli S. aureus	PDA/GO/AgNPs-Ti resulted in 99.8% and 99.6% effectiveness against E. coli and S. aureus, which is significantly higher than that of pure Ti and PDA/GO-Ti (<20%)	Cumulative effect	Clinic application	Xie et al., 2017 [47]
GO	Gold nanoclusters	S. aureus	GO and AuNCs resulted in 17% and <5% bacterial inactivation rates, compared with 34% for the GO-AuNP composite.	Cumulative effect	Clinic application	Zheng et al., 2019 [65]
rGO (montmorillonite modified, MTT)	Copper nanoparticles	E. coli S. aureus	MMT-rGO-CuNPs resulted in a >99% reduction in E. coli and S. aureus, compared to individual treatments which achieved no more than a 97% killing rate.	Unique surface property	Clinic application	Yan et al., 2019 [66]
GO	Red phosphorus (RP)	E. coli S. aureus	Ti-RP/GO resulted in >98% and >99.9% reduction under simulated sunlight and 808 nm for S. aureus and E. coli, compared with a 42% and 79% bacterial reduction caused by Ti-GO and Ti-RP alone.	Cumulative effect	Clinic application	Zhang et al., 2020 [67]
Graphene quantum dots (GQD)	AgNPs	E. coli S. aureus	GQD-AgNP resulted in >90% reduction for both S. aureus and E. coli under 450 nm, while GQD alone caused less than 30% and 40% reduction.	Cumulative effect	Clinic application	Mei et al., 2020 [68]
GO	Ni colloidal nanocrystal cluster (NCNC)	E. coli S. aureus	GO/NCNC resulted in 99.5% and 100% inhibition against S. aureus and E. coli, respectively, compared to 70–82% inhibition for individual components.	Cumulative effect	Clinic application	Du et al., 2022 [69]
GO	PVA (polyvinyl alcohol)	E. coli S. aureus	GO/PVA led to over 97% and 99% reduction in S. aureus and E. coli, respectively, under dual-wavelength light, compared to around 80% and 50% reduction by GO/PVA.	Cumulative effect	Clinic application	Li et al., 2021 [45]
rGO	pi-conjugated molecule containing five aromatic rings and two side-linked quaternary ammonium groups (piQA)	E. coli S. aureus	piQA-rGO rapidly removed most bacteria within 110 s compared to the inactivation time of piQA (10 min), while rGO resulted in just under a 30% loss of viability.	Unique surface property	Water purification	Wang et al., 2019 [56]
GO	ε-poly-L-lysine (PLL)	E. coli B. subtilis	GO-PLL retained 61% of E. coli and 53% of B. subtilis, which is significantly higher than the retention rates of 25% and 5% for the GO sponge without PLL, respectively.	Unique surface property	Water purification	Filina et al., 2019 [57]
rGO	Ag-AgBr nanoparticles	E. coli K12	Ag-AgBr/0.5% rGO resulted in 7 log reductions within 10 min, comparatively, Ag-AgBr and AgBr-rGO resulted in 7 and 5.5 log reductions in 40 min.	Cumulative effect	Water purification	Xia et al., 2016 [70]
GO	AgNP(silver nanoparticles)	E. coli S. Typhi S. aureus	The diameter of the highest inhibition zone for S. typhi was measured as 11.75 ± 0.96 mm. S. aureus: this value was measured as 9.88 ± 0.25 mm; E coli: this value was measured as 10.00 ± 0.41 mm, while GOQD used as negative control did not show any antibacterial activity	N/A	Water purification	Büşra et al., 2024 [71]
rGO	Starch/polyiodide	E. coli S. aureus	Starch/rGO/polyiodide nanocomposite resulted in inhibition zones of 22.2 ± 2.2 mm and 20.2 ± 0.9 mm for E. coli and S. aureus, respectively, whereas Starch/rGO alone did not exhibit any inhibition.	N/A	Antimicrobial food packaging	Narayanan et al., 2021 [60]
rGO	Pd-ZnO	P. aeruginosa K. pneumonia	Pd-RGO-ZnO exhibited antibacterial activity against a panel of human pathogens, including P. aeruginosa and K. pneumonia.	Unique surface property	Antimicrobial food packaging	Rajeswari et al., 2020 [61]
GO	Curcumin	Respiratory syncytial virus	Curcumin/GO resulted in 4 log reduction in viral titers, which was significantly higher than that caused by the individual components.	Cumulative effects	Other antimicrobial applications	Yang et al., 2017 [72]
GO	Polymeric N-halamine (PSPH)	E. coli S. aureus	GO-PSPH-Cl resulted in a 6.7 log reduction in S. aureus and an 8.1 log reduction in E. coli. Comparatively, GO and GO-PSPH resulted in <1.7 log and <2.7 log reduction of S. aureus and E. coli under the same condition.	Cumulative effects	Other antimicrobial applications	Pan et al., 2017 [73]

Note: rGO: reduced graphene oxide; GO: graphene oxide; N/A: Not applicable.

Antimicrobial application of graphene materials is a most-relevant scope that can be compatible with the synergistic improvements. However, it is important to consider the microbial viabilities in more detail. For example, AGCs may induce bacteria to enter a viable but non-culturable (VBNC) state during the inactivation phase. These bacteria remain virulent and can regain the ability to reproduce under appropriate conditions through a process known as resuscitation [74], resulting in subsequent therapeutic recovery or food cross-contamination. Most current studies have not detected VBNC bacteria when treated with AGCs. Similarly, including MRSA, a large number of resistant strains require more professional experiments to validate the possible synergistic inactivation induced by AGCs. Novel approaches such as bacterial gene expression and physiological metabolism can be assessed when comparing the bactericidal process of individual components with AGCs.

2.2. Medicinal Graphene-Based Composites for Cancer Therapy

Graphene nanosheets possess high drug loading, controlled release, and photothermal conversion capabilities under NIR, providing great potential for the application of graphene-based composites in cancer therapy. Doxorubicin and small interfering RNA (siRNA) co-delivery, based on GO-polyallylamine prepared through chemical synthesis, presented remarkable tumor suppression (62.3%) against hepatitis C virus-related liver cancer cells [75]. Comparatively, doxorubicin/GO-polyallylamine only slightly inhibited tumor growth (85.3%) in the short term (10 days), while other groups showed no inhibition of tumor cells at all [75]. Note that, usually, cancer typically develops due to the malignant transformation of tissue cells in the body, which may differ from the transplanted tumor cells in this study. In another study, noncovalently poly (ethylene glycol) (PEG)ylated nano-rGO loaded with Arg-Gly-Asp-based peptides (RGD) enabled efficient photothermal heating of solutions under low-power 808 nm radiation to target and further photoablate U87MG cells (cancer cells). U87MG cells incubated with nano-rGO-RGD and irradiated with 15 W/cm² NIR light for 8 min were destroyed. In contrast, cells treated with nano-rGO-RGD without irradiation, cells only irradiated with an 808 nm laser, and the control group all showed nearly 100% viability [76]. Hence, nano-rGO sheets could decrease the dosage required for both the photothermal agent (i.e., nano-rGO) and the drug, demonstrating environmentally friendly characteristics. Such synergistic effects were also observed in doxorubicin-loaded PEGylated nanographene oxide under 808 nm [77], nanosized rGO/PEGylation under 808 nm, rGO-polyethyleneimine-folic acid/doxorubicin [78], and indocyanine green-loaded polydopamine-rGO [79]. Notably, rGO has significantly higher drug loading efficiency for aromatic molecules compared to GO due to the reduction of oxygen-containing functional groups in GO during the rGO synthesis [78,80,81,82]. One of the benefits of using synergistic graphene complexes in cancer treatment is to lower the dosage of drugs needed for tumor suppression. Some of these graphene-based composites also have the capacity of targeted drug delivery. These findings make it favorable to develop a novel strategy with reduced negative health impacts, whereas the distribution, accumulation, and excretion of graphene-based composites in the body still need to be investigated.

2.3. Graphene-Based Catalysts

Global energy needs require novel catalysts with higher efficiency, lower costs, and better sustainability [83]. Highly efficient catalysts for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) are essential for achieving sustainable and efficient energy conversion/production or environmental purification [84]. As monolayers of sp² carbon atoms combine into a hexagonal lattice, graphene shows strong catalytic activity, representing a promising sustainable material for energy utilization. This is primarily attributed to its excellent electron capture and transport capacity, large specific surface area, and unique interactions with catalyst particles via noncovalent interactions (such as ionic interactions and π-π interaction) [85] or covalent bonds (e.g., C−C bonds) [86]. However, such catalytic capacity can be seriously affected if graphene single layers aggregate with very small interlayer spacing [87,88]. In this context, graphene material hybrids with selective compounds showing synergies as enhanced catalysts can be summarized separately into three different categories, photocatalysis, electrocatalysis, and chemical catalysis, as follows.

2.3.1. Graphene-Based Catalysts Revealing Synergistic Effects Through Photocatalysis

The photoinduced generation of holes in the valence band (VB) and excited electrons in the conduction band (CB) create a strong driving force for catalytic oxidation and reduction reactions, such as HER, OER, and CRR [84]. Under the light, photosensitizers (polymers [89], transition metal [90,91], or their oxides [92]) undergo charge separation, leading to the production of electrons and holes. However, the conducting efficiency of polymers, transition metals (such as Fe or Co), or their oxides are usually insufficient [93,94], due to the high degree of recombination process in electron (e)–hole (h⁺) pairs [95]. The addition of graphene planes into the composite could serve effective electron acceptors and suppress the recombination of electron–hole pairs. This allows rapid charge transfer from other counterpart compounds to the graphene layers, and the conjugated structure of graphene further accelerates charge transfer between graphene layers, which simultaneously improves the conductivity of graphene-based composites [92,96,97]. Hybridization with graphene and similar derivatives can also improve the photocatalytic activity by enhancing light absorption on the 2D planar structure of graphene [92]. Similarly, the synergistically enhanced photocatalytic properties of these graphene-based composites were also found to be associated with improved adsorbent absorptivity (e.g., pollutants) by providing abundant surface reaction sites [98]. Such advantages of graphene-based composites have evoked a number of research efforts to develop high-performance hybrid photocatalysts. For example, Fe and Co co-doped graphene was prepared through the π-π interaction of perylene diimide (PDI) within the self-assembled interface of iron–cobalt dual single-atom anchoring on nitrogen-doped graphene (FexCoy-NG). The obtained composite showed excellent photocatalytic activity for bisphenol A (98.5% degradation), surpassing that of NG/PDI (less than 50% degradation), Fe-NG/PDI (less than 90% degradation), and Co-NG/PDI (less than 90% degradation) under visible light irradiation. The high degradation performance of this composite is mainly attributed to its larger specific surface area, which improves pollutant adsorption capacity and facilitates transfer of electrons in the photocatalytic reaction [91]. In addition, Li et al. synthesized a hydrogel composite photocatalyst of 3D-2D-3D BiOI/porous g-C₃N₄/graphene (BPG) via a two-step hydrothermal method [99]. BPG exhibited the highest photocatalytic activity for degrading methylene blue (MB) under visible-light irradiation (λ ≥ 420 nm). The reaction rate constant (k = 0.472 h⁻¹) was 7.15 times higher than that of BiOI and 1.23 times higher than that of porous g-C₃N₄/graphene. The authors claimed that the synergistic effect in degradation can be ascribed to the shortened diffusion distance for photogenerated carrier transport and large contact area for rapid interfacial charge separation. Such improvements were also observed in the graphene–porphyrin metal–organic framework (MOF) composite [90], graphene-Fe/TiO₂ composite [92], magnetically separable CoFe₂O₄-graphene [100], copper-centered MOF supported graphene oxide [96], and cotton fabric coated with graphene/titanium dioxide nanocomposite [101]. However, it is conceivable that these graphene-based composites exhibit variability in their catalytic performances due to diverse interfacial contacts between graphene and other constituent components. Such contacts are crucial for the transfer and separation of photogenerated charge carriers [102].

2.3.2. Graphene-Based Catalysts Revealing Synergistic Effects Through Electrocatalysis

During the electrocatalytic process, graphene sheets within the graphene-base materials provide a large surface area, expose active and defective sites, and promote fast and mass electron transport. For example, the edge sites and defective structures of rGO serve as active sites for ORR. The 2D structure of rGO provides a high surface area, facilitating the easy transfer of electrolyte/O₂ to/from active sites on both sides. This characteristic led to the higher ORR and OER activity of CoFe₂O₄/rGO compared to CoFe₂O₄ or GO alone. The improved electrocatalytic action was evidenced by a notable rise in the current density for the OER of CoFe₂O₄/rGO (29.5 mA·cm⁻²), in contrast to CoFe₂O₄ (below 7.5 mA·cm⁻²) and rGO (below 15 mA·cm⁻²). In addition, the coupling between rGO and CoFe₂O₄ plays an important role in the OER process for the CoFe₂O₄/rGO nanohybrid. The catalytic activity of CoFe₂O₄/rGO for both ORR and OER is significantly higher than that of the mixture of rGO and CoFe₂O₄. This indicated that closer contact between CoFe₂O₄ and rGO promotes electronic conduction, ultimately enhancing electrocatalyst performance [103]. Similarly, high electrocatalytic OER activity was achieved by introducing graphene carbon dots (GCDs) to the finely tailored FeNi₃ alloy. The dendrite-like FeNi₃@GCDs were synthesized via a facile hydrothermal approach, with enlarged active areas, significantly enhanced electrical conductivity and a strong synergistic coupling effect. This led to an extraordinary OER performance with an overpotential of 238 mV (at a current density of 10 mA·cm⁻²) and a small Tafel slope of 48.7 mV·dec⁻¹ [104]. It is important to note that the electrocatalytic performance of graphene-based composites is highly dependent on their stability. Therefore, preventing graphene aggregation is a vital consideration.

2.3.3. Graphene-Based Catalysts Revealing Synergistic Effects Through Chemical Catalysis

In chemical reaction processes, graphene nanosheets support or adsorb counterpart components through interfacial interactions to form new bonds, activating catalytic actions or preventing aggregation to increase active sites. Large surface areas and the oxygen groups of GO sheets facilitate the formation of Co-OH complexes through the direct interaction of Co species with nearby hydroxyl groups or through the dissociation of H₂O with Co²⁺. The formation is proposed to accelerate the heterogeneous activation of peroxymonosulfate, which generates sulfate radicals to degrade pollutants [105]. The resulting catalyst exhibited synergistic catalytic performance in degrading Orange II in water (100% degradation) in 4 min, which is significantly higher compared to the treatments using bare Co₃O₄ (approximately 10% degradation) and GO (almost 5% degradation). In the Fenton-like oxidation of sulfonamides, which are widely used as antibiotics and are harmful to the environment and human health, the catalytic efficiency of goethite (Gt)-rGO (98.0% degraded) with an optimal rGO content of 6% was significantly higher than rGO (24.5% degraded) or Gt (44.0% degraded). The synergistic catalytic effects were attributed to the increased disorder of rGO layers and more exposed sites for H₂O₂ activation. Gt-rGO exhibited fast Fe (III)/Fe (II) cycling through Fe-C coordination, which generated -OH radicals by Fenton reaction for the degradation of sulfonamides. It should be noted that excessively high GO loading would reduce the exposure of Gt, hinder electron transfer, and decrease catalytic efficiency [106]. Graphene-based composites also exert a synergistic effect by physically adsorbing pollutants through π-π stacking interaction, which in turn further degrades pollutants by chemical oxidation. By this way, 4-nitrophenol (4-NP), a potential carcinogen, teratogen, and mutagen, was strongly absorbed and reduced by rGO surface alloyed with Au and Cu. The Au₃-Cu₁/rGO nanocatalyst synthesized by the deposition–precipitation method showed the highest kapp value of 96 × 10⁻³·s⁻¹, which is nearly 9 times higher than that of Au (kapp = 11 × 10⁻³·s⁻¹) and approximately 14 times higher than that of Cu (kapp = 7 × 10⁻³·s⁻¹) due to the enhanced electronic communication and strong adsorption between 4-NP and Au-Cu/rGO, facilitating the direct reduction of 4-NP [23]. The authors innovatively studied the synergistic effect of Au-Cu nanoparticles and rGO based on density functional theory. They found that the adsorption energy of Au-Cu/rGO is much higher than that of pure rGO and Au-Cu, and the bond lengths in the Au-Cu/rGO system are changed. This, to some extent, explains the higher catalytic activity of Au-Cu/rGO compared to other catalysts.

It is worth mentioning that the formation of the interface and the contact angle between graphene and non-graphene components plays an important role in synergistic catalytic effects. Non-graphene components are activated by graphene through charge transfer and hole formation across the interface, which also ensures strong adhesion between the components. The contact angle, the ratio of interfacial area to surface area between graphene and non-graphene materials, is another factor that affects the dispersion of the active component. These factors need to be considered during material processing to obtain the anticipated synergistic effect. A detailed overview of the graphene-based catalysts has been outlined in Table 2.

Table 2. Representative studies demonstrating significant synergistic catalytic effects in graphene-based composites.

Graphene Composites	Synergistic Components	Reaction	Synergistic Catalytic Capacity	Synergistic Mechanisms	Applications	Reference
Nitrogen-doped graphene (NG)	Fe_xCo_y/perylene diimide (PDI)	Degradation of Bisphenol A (BPA)	Fe₀.₂Co₀.₈-NG/PDI degraded 100% of BPA, while NG/PDI, Co-NG/PDI, and Fe-NG/PDI degraded only 50%, 65%, and 90% of BPA, respectively.	Cumulative effect	Photocatalysis	Liu et al., 2023 [91]
Graphene	Fe/TiO₂	Degradation of methyl Orange	Graphene-0.5Fe/TiO₂ composites have a 10-fold enhancement in photocatalytic activity compared to pure TiO₂, surpassing GR-TiO₂ (six times) and Fe-TiO₂ (two times).	Fast electron transfer	Photocatalysis	Khalid et al., 2012 [92]
N-doped reduced graphene oxide (NRG)	SnS₂/polyaniline	Degradation of Cr (VI)	The reaction rate constant (k) for photocatalytic reduction in Cr (VI) using polyaniline/SnS₂/NRG2% is 3.8, which is higher than that of SnS₂ (0.8), SnS₂/NGR (1.9), and SnS₂/polyaniline (2).	Cumulative effect	Photocatalysis	Zhang et al., 2018 [107]
Graphene	Co-Fe₂O₄	Degradation of methylene blue (MB)	CoFe₂O₄-G degrades most of MB under visible-light irradiation at 25 °C, while pure CoFe₂O₄ hardly degrades MB.	Cumulative effect	Photocatalysis	Fu et al., 2012 [100]
Graphene	TiO₂	Degradation of MB	G-TiCl₃ led to an 89.13% and 78.15% decrease in MB concentration when irradiated with UV and sunlight, respectively. In comparison, G reduced MB by 6.7% and 6.5%, while TiCl₃ reduced MB by 34.5% and 14.2%.	Cumulative effect	Photocatalysis	Karimi et al., 2015 [101]
NG	Fe oxide/Fe hydroxide	Degradation of antibiotics (Chloramphenicol sodium succinate, CAP)	The Fe oxide/Fe hydroxide/N-rGO hybrid nanocomposites degraded around 62.5% of CAP under visible light irradiation during 150 min, in contrast to pure Fe oxide/Fe hydroxide (around 5%) or N-rGO layers (under 15%).	Fast electron transfer	Photocatalysis	Ivan et al., 2023 [108]
GO	Copper-centered metal (MOF)	Hydrogen evolution reaction (HER) Oxygen evolution reaction (OER) Oxygen reduction reaction (ORR)	The electroactive surface area of GO/Cu-MOF is 20 times higher than that of the bare electrode, while that of Cu-MOF is 4 times higher, with almost no increase in GO.	Cumulative effect	Electrocatalysis	Jahan et al., 2013 [96]
rGO	Iron–porphyrin metal–organic framework ((Fe-P) nMOF)	ORR	The redox current of G-(Fe-P)_nMOF increased nearly 10-fold compared to bare GC, while (Fe-P)_nMOF increased 2-fold.	Cumulative effect	Electrocatalysis	Jahan et al., 2012 [90]
rGO	CoFe₂O₄	ORR OER	The current density for the OER of CoFe₂O₄/rGO is significantly higher at 29.5 mA·cm² compared to CoFe₂O₄ (below 7.5 mA·cm⁻²) and rGO (below 15 mA·cm⁻²).	Fast electron transfer	Electrocatalysis	Bian et al., 2014 [103]
rGO	Boron nitride nanosheets (BNNSs)	Li₂S conversion	BNNSs/rGO exhibits the lowest onset potential (−0.41 V) compared with BNNSs + rGO (−0.32 V), rGO (−0.28 V) and BNNSs (−0.26 V) electrodes.	Cumulative effect	Electrocatalysis	Yang et al., 2023 [109]
GO	Co₃O₄	Degradation of Orange II	GO-Co₃O₄ degraded Orange II in water (100% degradation) in a very short time of 4 min, while bare Co₃O₄ (approximately 10% degradation) and GO (nearly 5% degradation) did not.	Cumulative effect	Chemical catalysis	Shi et al., 2014 [105]
rGO	Au-Cu	Degradation of 4-nitrophenol (4-NP)	The Au₃-Cu₁/rGO nanocatalyst showed the highest k_app value of 96 × 10⁻³·s⁻¹, which is nearly 9 times higher than that of Au/rGO (k_app = 11 × 10⁻³·s⁻¹) and approximately 14 times higher than that of Cu/rGO (k_app = 7 × 10⁻³·s⁻¹).	Cumulative effect	Chemical catalysis	Rout et al., 2017 [23]
Graphene	C₃N₄	Production of cyclohexanone	G-C₃N₄ (with ~1.2 wt% graphene) provides the highest yield (5.4%) for cyclohexanone, while graphene or C₃N₄ alone cannot produce any cyclohexanone.	Fast electron transfer	Chemical catalysis	Chen et al., 2016 [110]

Note: rGO: reduced graphene oxide; GO: graphene oxide.

2.4. Graphene-Based Composites with Improved Mechanic Properties

Graphene-based composites have been extensively investigated for applications requiring improved hardness, elasticity, and other mechanical properties, including those in vehicle manufacturing, aerospace, construction, and defense sectors [111]. Owing to their lightweight nature, corrosion resistance, facile processing, and electromagnetic interference shielding capability, graphene-based composites represent a highly promising sustainable material. A single layer of graphene is mechanically strong with a Young’s modulus of approximately 1 TPa and a strength of around 130 Gpa [112]. However, simply adding graphene to the material matrices did not improve the mechanical properties as expected. This result can mainly be ascribed to the agglomeration issue, which may have been associated with the point of failure during testing due to strong van der Waals forces and its high specific surface area, as well as the weak bonding between graphene and the matrix [113]. The latter rendered it incapable of performing effective stress transfer. Therefore, studies have found that the synthesis of hybrid composites based on graphene materials could be a feasible solution [114,115,116]. A more specific synergistic mechanism can be summarized based on the above literature as follows: First, the strong interfacial interactions between graphene-based composites and fillers (such as metals) through covalent bonds or non-covalent interactions (such as hydrogen bonds and van der Waals forces) help build an interconnected network. This prevents the stacking and face-to-face agglomeration of graphene sheets. Secondly, the architecture inhibits slipping under tensile stress through a “mechanically locked structure”, which contributes to the overall enhancement of the composite’s mechanical attributes. In this manner, the mechanical properties of hybrid composites can be further improved. For example, a synergistic effect arises from the scroll-like structure produced by combining carbon nanotubes (CNTs) with GO. The GO–CNT/poly (vinyl alcohol) composite films with retained ductility show superior mechanical properties compared to PVA composite films enhanced solely by GO or CNT. The tensile strength and Young’s modulus of the composites are increased by 148% and 132% compared to pure PVA, respectively. They are also significantly higher than the combined percent improvement of CNT/PVA and GO/PVA (yield strength: 6% + 29%; Young’s modulus: 3% + 13%) [114]. Such synergistic effects were also observed in a GO-Ag co-dispersing nanosystem [116] and polymer nanocomposites consisting of graphene oxide and carbon nanotubes [111,117,118,119,120]. Increased material hardness has also been realized through graphene incorporation. For instance, when graphene was integrated into a Cu matrix via pulse reverse electroplating, this improved hardness by 2.5 GPa and modulus by 137 GPa, which are 2 and 1.2 times higher than bulk Cu, respectively. This enhanced effect can also be observed in Cu-graphene nanocomposites [121]. Most other studies, however, hardly test the hardness of graphene alone. It is worth noting that the mixture ratio plays a key role in controlling the reinforcing ability of composite materials [122,123]. Furthermore, it is important to test the mechanical properties of these materials under extreme or simulated conditions, such as zero gravity in a space environment, to further evaluate their effectiveness.

2.5. Graphene-Based Conductive Composites

Today’s escalating demands for renewable energy resources propel research into efficient energy storage systems, such as batteries and supercapacitors. The surface modifiability, ductility, conductivity, and physical stability of graphene make it possible to use graphene-based composites as high-capacity renewable energy sources [124,125,126]. The main challenge is to ensure adequate electrolyte diffusion across the entire surface area of graphene, especially at high current densities [127]. To alleviate the restacking of graphene, it is available to combine with metal oxides [128], chalcogenides [129], and conducting polymers [130]. For example, embedding small carbon black nanoparticles within the narrow interstices between graphene nanosheets ensures high chemical stability and further accumulates more connected pathways of electron flow (Figure 3A-1,2), resulting in augmented initial conductivity of the composite at each ultimate strain (Figure 3A-3) [131].

Figure 3. Structural change for carbon black-TPU, graphene-TPU (A-1), and graphene/carbon black 3:7-TPU composites (A-2) before and after stretching and their initial conductivity versus ultimate strain (A-3) [131]; Copyright © 2022, Taylor & Francis. The formation of rGO/MnFe₂O₄ binary and rGO/MnFe₂O₄/PPy ternary hybrids (B-1). Calculated Cs of corresponding hybrids at different scan rates (B-2) and Nyquist plots of PPy, MG binary, and PPy/MG ternary hybrids showing and high-frequency regions (B-3). Reproduced with permission [124], Copyright © 2019, Elsevier.

In addition, the combination of graphene-supported manganese ferrite microspheres (MG) and a conductive polymer (polypyrrole, PPy) via co-precipitation method (Figure 3B-1) showed maximum capacitive performance (147.2 F/g at scan rate of 10 mV/s), while the individual capacitance of MG or PPy is 22.1 F/g and 59.3 F/g, respectively (Figure 3B-2) [124]. As observed in the low-frequency region of the Nyquist plot (characterized by straight-sloping lines (Figure 3B-3), the slope of the straight lines increases with a higher PPy ratio in the MG composite, indicating reduced diffusion resistance. This behavior demonstrates an improvement in the capacitive performance of the resulting hybrid material. Therefore, this synergistic effect is attributed to improved electron transfer and shortened diffusion paths, making MG/PPy a promising candidate for energy storage in supercapacitors. In another study, the synergistic coupling of titanium carbonitride nanocubes with GO using a deposition method showed an 800-fold fluorescence enhancement. This enhancement was attributed to integrated hotspots with enhanced electromagnetic fields compared to using only GO (30-fold) or titanium carbonitride nanocubes (400-fold) [132]. The high loading capacity of the conductive filler boosts the percolation pathway but can result in a porous final composite with somewhat diminished mechanical properties. Balancing high electrical conductivity and mechanical strength is therefore necessary in material development.

It is evident that combining graphene with selected functional materials can significantly enhance key properties such as initial electrical conductivity, capacitive performance, and loading capacity. These improvements demonstrate the distinct advantages and potential of graphene-based composites in conductive applications, further contributing to sustainable technological development.

2.6. Graphene-Based Sensors

Graphene-based sensors, renowned for their acute sensitivity and specificity, have been extensively studied in recent years. A stable and accurate sensor for detecting zearalenone (ZEA), a non-steroidal estrogenic mycotoxin in food, was developed by reducing and modifying oxidized graphene nanoribbons (GNRs) and AuNPs on a glassy carbon electrode using an electrodeposition technique [133]. The as-prepared sensor showed a wide linear range (1–500 ng·mL⁻¹) and a low detection limit (0.34 ng·mL⁻¹) after incorporating molecularly imprinted polymer (MIP), known as one of the most efficient recognition elements for electrochemical sensors (Figure 4A). A similar synergistic effect was observed in the β-cyclodextrin-GO system. As shown in Figure 4B, neither GO nor β-CD alone enhanced the electrocatalytic activity of the bare screen-printed carbon electrode (SPCE) (reduction peaks remained around −0.73 V); however, when the β-CD/GO composite was introduced to the SPCE, the reduction peak current of nitrobenzene (NB) increased 2-fold, accompanied by a positive shift in the reduction potential. This enhanced electrocatalytic activity demonstrates the synergistic effect between β-CD and GO on the SPCE [134]. Furthermore, the reaction products exhibited an anodic peak (II) at 0.03 V and a cathodic peak (III) at 0.06 V, corresponding to the redox behavior between phenylhydroxylamine and nitrosobenzene, which contributes to the elimination of nitrobenzene contamination [135].

For microorganism detection, a biosensor assembled with graphene-based nanocomposites, metals, or conducting polymer, along with aptamer probes, can differentiate the target microorganisms directly from the complex environmental background. As is depicted in Figure 4C-1, a GO-wrapped Fe₃O₄-Au nanostructure aptamer sensor was developed for detecting Vibrio parahaemolyticus in spiked salmon samples [134]. This hybrid sensor employs dual aptamers acting as capture and sensing probes, eliciting a substantially amplified Surface-Enhanced Raman Scattering (SERS) response specifically toward Vibrio parahaemolyticus (Figure 4C-2). The synergistic electromagnetic enhancement by AuNPs combined with GO was due to the high adsorption and charge transfer effect on the graphene basal plane, leading to its high specificity and sensitivity with a detection limit of 14 CFU/mL. Similar observations for microorganism detection were also reported including polypyrrole/pyrrolepropylic acid/rGO-based immunosensors [136], ZnFe₂O₄/rGO [135], and MoS₂@graphene quantum dots/ITO (Figure 4D) [137].

Strain sensors with high sensitivity, a broad sensing range, significant stretchability, and low voltage operation are pursued for applications in health monitoring and biomedicine. Zhou et al. developed a slit and shell-like strain sensor that exhibits extensive stretchability (680%), superior electrical conductivity (1521 S·cm⁻¹), high sensitivity (≈107 at 120% strain), rapid response time (<30 ms), and excellent reproducibility over 2000 cycles [138]. This strain sensor was covered with frAGCented graphene sponges (FGS) and further embedded in poly (styrene-block-butadiene-block-styrene) (SBS) for increased stretchability and easy absorption of Ag ions. FGS/SBS/Ag possessed a low gauge factor versus strain (1–5 × 10⁵), while that of FGS/SBS and Ag/SBS reached 10⁶–10⁷ and 10⁸–10⁹, respectively (Figure 4E). The potential synergistic mechanism is described as follows: (1) variations in microcrack junctions in the silver oxide layer (cracking mechanism) and the overlapping area of neighboring FGS (disconnection mechanism) lead to enhanced sensitivity; and (2) the FGS tended to bridge the disconnected network of silver oxides under tensile strain.

Figure 4. Examples of graphene-based composites as sensors: CV measurements of a SERS aptamer-based sensor on GO-wrapped MIP/AuNPs/GCE for zearalenone determination CV measurements of bare GCE (a), rGNRs/GCE (b), AuNPs/GCE (c), AuNPs/rGNRs/GCE (d), MIP/AuNPs/rGNRs/GCE before template removal (e), MIP/AuNPs/rGNRs/GCE after elution (f), and MIP/AuNPs/rGNRs/GCE after adsorption of 150 ng·mL⁻¹ ZEA solution (g) (A). Reproduced with permission [133], Copyright © 2023, Elsevier. CV (Cyclic voltammetry) response of bare SPCE (a), β-CD/SPCE (b), GO/SPCE (c), and GO/β-CD/SPCE (d) (B). Reproduced with permission [134], Copyright © 2017, Elsevier. Schematic of SERS aptasensor based on GO-wrapped Fe₃O₄@Au nanostructures (C-1), and the SERS response spectra of this aptasensor in the presence of different concentration of V. parahaemolyticus (C-2) [138], Copyright © 2017, Springer. EIS studies of (i) ITO, (ii) MoS₂/ITO, (iii) MoS₂@GQDs/ITO, (iv) aAFB₁/MoS₂/ITO, and (v) aAFB₁/MoS₂@GQDs/ITO electrodes (D). Reproduced with permission [137], Copyright @ 2020, Springer. Gauge factor versus strain for SBS/Ag, FGS/SBS, and FGS/SBS/Ag composite (E). Reproduced with permission [139], Copyright © 2017,Wiley.

Owing to the intrinsic superior properties of graphene, graphene-based composites have led to remarkable synergistic improvements in sensor performance. These enhancements, which include both elevated sensitivity and reinforced specificity, offer versatile opportunities for optimizing sensor functionality and diversifying material sources.

2.7. Graphene-Based Electromagnetic Interference (EMI) Shielding

With the advancement of next-generation electronic information technologies, electronic devices have brought considerable convenience while also generating electromagnetic waves that propagate in the form of radiation and heat. These emissions have raised concerns over potential health risks, environmental pollution, and the leakage of sensitive electromagnetic information. Consequently, the development of high-performance EMI shielding materials has become particularly critical to mitigate these challenges.

The incorporation of graphene and carbon nanotube fillers offers a promising strategy for optimizing the electrical, mechanical, thermal, and EMI shielding properties of nanocomposites. At the same filler loading, the composite with a graphene–MWCNT (multi-walled carbon nanotube) ratio of 1:3 achieved the highest electrical conductivity of 1.91 × 10⁻¹ S/cm at a hybrid filler loading of 10 phr. This remarkable enhancement in electrical conductivity directly contributed to an excellent EMI shielding effectiveness of −34 dB in the X-band (8.2–12.4 GHz). Additionally, it exhibited the highest tensile strength and tensile modulus, demonstrating overall significant synergistic effects between graphene and MWCNT [115].

Similarly, Erzhen Z et al. [140] reported a notable synergistic effect on graphene and CNTs. By incorporating only 20 wt% CNTs into the graphene film, the electrical conductivity was significantly enhanced from 1.78 × 10⁵ S/m to 2.74 × 10⁵ S/m, and the thermal conductivity increased markedly from 510 W·m⁻¹·K⁻¹ to 1154 W·m⁻¹·K⁻¹. Furthermore, the macroscopically assembled graphene–CNT hybrid film (with 20% loading) exhibited an improved EMI shielding effectiveness of ~60 dB, representing a substantial increase of approximately 10 dB compared to that of pure graphene film (~50 dB). The discovery of this synergistic behavior provides a promising strategy for designing advanced materials with superior electrical and thermal conductivity, as well as enhanced EMI shielding performance.

3. Synergistic Mechanisms in Graphene-Based Composites

In the preceding sections, graphene-based composites have shown synergistic effects in various applications, supported by experimental evidence. Although these mechanisms derive from the innate properties of graphene derivatives or their interactions with the supplementary components, a systematic summation of the synergistic mechanisms is not comprehensive. Consequently, we proposed four possible common mechanisms that might be useful to explain synergistic effects on distinctive occasions.

3.1. Unique Surface Property

The nanostructure of graphene or graphene oxide provides an elevated surface-to-volume ratio as well as a large active surface area. On the one hand, this enables graphene sheets to gather other associated components (e.g., metals or metal oxides nanoparticles) locally, greatly increasing their concentration. On the other hand, target microorganisms or reactants can be adsorbed on the graphene surface more tenaciously, either through covalent bonds or noncovalent interactions, as opposed to when graphene or non-graphene components act individually. The sharp edges of the graphene surface sheet also directly penetrate microbial cells. These advancements could enhance the performance of graphene-based composites in antimicrobial activities, cancer therapy, catalysis, and sensing.

3.2. Enhanced Stability and Active Areas

Graphene sheets enable the uniform distribution of combined compounds on their surface structure. This can form co-supportive networks due to strong interfacial adhesion between graphene and the combined materials. This significantly diminishes the tendency of graphene sheets and other components (e.g., Ag), thereby increasing the reaction activities in binding areas. This synergistic mechanism may exist in graphene-based composites with bolstered antimicrobial capacity, enhanced catalytic action, and improved or advanced electronic devices.

3.3. Fast Electron Transfer

Fast electron transfer in graphene-based composites also plays a key role in generating synergistic effects. The graphene plane facilitates the electron transfer from noble metals or conducting polymers, resulting in improved conductivity and increased oxidative capacity, superior to that afforded by either graphene or non-graphene components alone. The outcomes of such actions improve conductivity, antimicrobial activities caused by oxidation, sensitivities in electronic devices and sensors, catalysis, etc.

3.4. Cumulative Effects

Often, the properties of graphene-based composites are enhanced by the simultaneous actions of two or more of the aforementioned mechanisms, known as the cumulative effects. This may significantly improve material performance due to fortification of multiple individual factors. A summary of synergistic mechanisms between graphene planes with different components is illustrated in Figure 5.

4. Conclusions, Challenges and Future Perspectives

Synergistic effects in graphene-based composites have been observed during antimicrobial treatments, cancer therapy, catalysts, mechanical properties, electronic devices, and sensor applications. Each combination of graphene and non-graphene components exhibits a specific synergistic extent and a niche application, with overall improvements shown over singular treatments and potential effectiveness toward sustainability. In this review, we elucidate the mechanisms of various graphene-based composites associated with their remarkable hybridization characteristics in specific applications. Moreover, we proposed four primary synergistic mechanisms, broadly categorized as follows: (1) synergistic effect induced by unique surface properties of graphene-based composites; (2) synergistic effect induced by enhanced stability and active areas of graphene-based composites; (3) synergistic effect induced by fast electron transfer; and (4) cumulative effects of the above mechanisms generated by graphene nanosheets and the counterpart materials. Therefore, more theoretical work and solid experimental research is crucial to demystify these mechanisms further.

Despite copious studies on graphene and related materials, the market for these revolutionary substances is still embryonic. Based on the endorsement of granted patents, the commercialization of graphene-based composites is expected to expand significantly, leading to increased revenue and production scale in the next 5–10 years [136]. Therefore, developments and applications of graphene-based composites will soar with the upgrading of massive graphene production systems and reduced costs.

Future work shall focus on tackling the major obstacles to the application of graphene-based materials in health-relevant fields, particularly biocompatibility. Generally, graphene-based composites with small and individual graphene sheets, inclusive of capping agents or with controlled-release mechanisms, are more readily internalized by macrophages, excreted, or efficiently degraded [55,135,141]. Therefore, some studies have commenced the tailoring of graphene-based composites with dispersion and separation properties to effectively increase the active sites of graphene sheets with higher performance. However, few have directly tackled the cytotoxicity of graphene nanosheets or metals within graphene-based composites in animal models. The advancement of prototypes with attenuated toxicity will pave the way for broader applications. Additionally, graphene variability in terms of layer count, defect densities, and sizes leads to performance inconsistencies in composites, posing a challenge for quantitative design and industrial-scale and high-quality production. These above-mentioned obstacles shall be properly handled in future studies.

Furthermore, as large-scale usage of graphene-based materials looms, their biodegradability, recycling options, and long-term impacts on human health and ecosystems necessitate consideration. Quantitative analysis is guaranteed for LCA and material consumption estimations when synergistic effects are employed during material design and fabrications. Regulatory frameworks must also adjust to accommodate a recommended graphene-based material dosage for deployment in biomedicines, chemical industries, foods, or water treatments, etc. [56].

Funding

This research received no external funding.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Not applicable.

Acknowledgments

Authors acknowledge the support of the 2115 Talent Development Program of China Agricultural University.

Conflicts of Interest

The authors declare no conflict of interest.

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Figure 1. Publication statistics on graphene-based composites in different application areas from 2010 to 2023 (A); data obtained from Web of Science. Scheme of potential applications of graphene-based composites with improved performance based on the synergistic effects (B).

Figure 2. Examples of graphene-based composites in antimicrobial applications: Antibacterial efficacy of ZnO/GO compared ZnO or GO alone (A-1) and the morphology of the bacterial membrane treated with spindle-shaped GO, ZnO and ZnO/GO composites (A-2). Reproduced with permission [36], Copyright © 2018, Elsevier. Wound healing effect of MGO0.5-TPU (B). Reproduced with permission [39], Copyright © 2020, Elsevier. PVA/Cu/graphene nanocomposite antiviral activity (C-1) and transparency of dip-coated tempered mobile screen *: Significance is defined as p < 0.05; ***: Significance is defined as p < 0.001. (C-2). Reproduced with permission [40], Copyright © 2021, American Chemical Society.

Figure 5. Proposed synergistic mechanisms between graphene planes and different components for materials performance. Created with BioRender.com.

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Xiao, J.; Gao, X.; Xu, J.; Tan, J.; Zhang, X.; Zhang, H. Unveiling the Synergistic Effects in Graphene-Based Composites as a New Strategy for High Performance and Sustainable Material Development: A Critical Review. Sustainability 2025, 17, 10058. https://doi.org/10.3390/su172210058

AMA Style

Xiao J, Gao X, Xu J, Tan J, Zhang X, Zhang H. Unveiling the Synergistic Effects in Graphene-Based Composites as a New Strategy for High Performance and Sustainable Material Development: A Critical Review. Sustainability. 2025; 17(22):10058. https://doi.org/10.3390/su172210058

Chicago/Turabian Style

Xiao, Jie, Xingxing Gao, Jie Xu, Juzhong Tan, Xuesong Zhang, and Hongchao Zhang. 2025. "Unveiling the Synergistic Effects in Graphene-Based Composites as a New Strategy for High Performance and Sustainable Material Development: A Critical Review" Sustainability 17, no. 22: 10058. https://doi.org/10.3390/su172210058

APA Style

Xiao, J., Gao, X., Xu, J., Tan, J., Zhang, X., & Zhang, H. (2025). Unveiling the Synergistic Effects in Graphene-Based Composites as a New Strategy for High Performance and Sustainable Material Development: A Critical Review. Sustainability, 17(22), 10058. https://doi.org/10.3390/su172210058

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Unveiling the Synergistic Effects in Graphene-Based Composites as a New Strategy for High Performance and Sustainable Material Development: A Critical Review

Abstract

1. Introduction

2. Synergistic Effects Observed in Graphene-Based Composites

2.1. Antimicrobial Graphene-Based Composites (AGCs)

2.1.1. AGCs Revealing Synergistic Effects for Clinic Application

2.1.2. AGCs Revealing Synergistic Effects for Water Purification

2.1.3. AGCs Revealing Synergistic Effects for Packaging Development

2.1.4. AGCs Revealing Synergistic Effects on Other Antimicrobial Applications

2.2. Medicinal Graphene-Based Composites for Cancer Therapy

2.3. Graphene-Based Catalysts

2.3.1. Graphene-Based Catalysts Revealing Synergistic Effects Through Photocatalysis

2.3.2. Graphene-Based Catalysts Revealing Synergistic Effects Through Electrocatalysis

2.3.3. Graphene-Based Catalysts Revealing Synergistic Effects Through Chemical Catalysis

2.4. Graphene-Based Composites with Improved Mechanic Properties

2.5. Graphene-Based Conductive Composites

2.6. Graphene-Based Sensors

2.7. Graphene-Based Electromagnetic Interference (EMI) Shielding

3. Synergistic Mechanisms in Graphene-Based Composites

3.1. Unique Surface Property

3.2. Enhanced Stability and Active Areas

3.3. Fast Electron Transfer

3.4. Cumulative Effects

4. Conclusions, Challenges and Future Perspectives

Funding

Institutional Review Board Statement

Informed Consent Statement

Data Availability Statement

Acknowledgments

Conflicts of Interest

References

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