Macromol

Alternating glycopolymers bearing periodically arranged pendant carbohydrate residues were synthesized by reversible addition–fragmentation chain transfer (RAFT) copolymerization of maltose-containing vinyl ether (MalVE) and ethyl maleimide (EtMI). The resulting trithiocarbonate-terminated polymers were subsequently converted into thiol-terminated glycopolymers through post-polymerization end-group transformation. These structurally well-defined alternating glycopolymers were immobilized onto gold nanoparticles (AuNPs) via Au–S interactions to construct glycopolymer-functionalized glycointerfaces. Surface functionalization of the AuNPs was confirmed by an increase in hydrodynamic diameter from approximately 42 to 59 nm after polymer immobilization. The resulting glycopolymer-functionalized AuNPs exhibited concentration-dependent lectin-mediated aggregation behavior in the presence of concanavalin A, accompanied by characteristic red shifts and broadening of the localized surface plasmon resonance (LSPR) band arising from multivalent carbohydrate–lectin interactions at the nanoparticle interface. Although the apparent association constants obtained for free alternating glycopolymers using fluorescently labeled lectin cannot be directly compared with those obtained from LSPR-based aggregation assays of AuNP-immobilized glycopolymers, the values increased from the order of 10⁵ L mol⁻¹ in solution to the order of 10⁷ L mol⁻¹ at the nanoparticle interface. This trend suggests that immobilization onto AuNPs enhances multivalent carbohydrate–lectin interactions through multivalent presentation of the glycopolymer chains at the nanoparticle interface. As a control experiment, peanut agglutinin (PNA), which does not recognize maltose residues, was added to the glycopolymer-functionalized AuNPs. No significant LSPR shift or spectral broadening was observed, indicating that nanoparticle aggregation was not induced by nonspecific lectin addition but arose from specific interactions between maltose residues and Con A. Quantitative analysis suggested that polymer chain length may influence the aggregation behavior. These results demonstrate that alternating glycopolymers provide a useful platform for constructing sequence-regulated glycointerfaces and for investigating multivalent biomolecular interactions at nanoparticle surfaces. Full article

Hepatocellular carcinoma (HCC) is among the most prevalent and lethal malignancies worldwide, with limited therapeutic outcomes due to systemic toxicity and suboptimal efficacy of conventional chemotherapeutics such as doxorubicin (DOX). In this study, we formulated and standardized DOX-loaded chitosan/poly (lactic-co-glycolic acid) nanoparticles (DLCNs) via a nanoprecipitation method and evaluated their therapeutic potential in a diethylnitrosamine (DEN)-induced Wistar rat model of HCC. Physicochemical analyses confirmed nanoscale size, favorable zeta potential, and high encapsulation efficiency, while Fourier-transform infrared spectroscopy (FTIR) verified polymer–drug interactions. Biochemical analysis revealed that DLCNs significantly normalized elevated liver function markers (Aspartate aminotransferase (AST), alanine aminotransferase (ALT) and alkaline phosphatase (ALP), restored serum α-fetoprotein (AFP) to near-control levels, and reduced lipid peroxidation compared with free DOX and DEN controls. Antioxidant profiling demonstrated marked recovery of superoxide dismutase (SOD), catalase (CAT), and glutathione peroxidase (GPx), indicating restoration of hepatic redox balance. Histopathological evaluation further corroborated these findings, showing recovery of hepatic lobular architecture and reduction in necrosis and inflammatory infiltrates in DLCN-treated Wistar Albino rats, while free DOX groups exhibited hepatocellular damage. Overall, the results demonstrate that encapsulating DOX in a chitosan/PLGA nanocarrier improves therapeutic efficacy, mitigates hepatotoxicity, and enhances antioxidant defense, establishing DLCNs as a favorable candidate for HCC. Full article

Bone loss in the maxillofacial region arises from multiple causes, including periodontal disease, trauma, surgical procedures, infection, congenital anomalies, and cancer. Traditional treatment relies on bone grafting, either alone or in combination with biomaterials. Advances in tissue engineering have introduced synthetic or natural scaffolds to mimic the mineralized bone matrix. Natural scaffolds offer excellent biocompatibility and similarity to native tissue but often lack sufficient mechanical strength and exhibit poor degradation rates. Synthetic scaffolds provide tunable porosity and mechanical stability; however, their biological inertness makes them poor sources of osteogenic signaling. A key factor in the success of any scaffold is its interaction with the host immune system. Upon implantation, the innate immune response is initiated, with neutrophils and macrophages being the first cells to contact the scaffold. Macrophage polarization toward proinflammatory (M1) or anti-inflammatory (M2) phenotypes determines whether the microenvironment favors inflammation or remodeling. The adaptive immune response also plays a critical role: T and B lymphocytes may promote tolerance and integration through Th2/Treg pathways and antibody-mediated regulation, or they may trigger chronic inflammation and rejection through Th1/Th17 activation. This review examines the natural and synthetic materials used for bone remodeling and their biological properties. It then outlines the sequence of immune events occurring from the moment a scaffold is implanted to its potential integration or failure. Finally, this study highlights the relevance of cellular models and in vitro assays for the early evaluation of immunogenicity and biocompatibility, which are essential for optimizing scaffold design and improving outcomes in maxillofacial bone regeneration. Full article

Cysteine proteases (bromelain, ficin, and papain) are widely used in biotechnology and medicine, but their application is limited by rapid autolysis and oxidative inactivation. This study aimed to develop effective supports for these enzymes based on graft copolymers of sodium alginate and poly(N-vinylpyrrolidone) (SA-g-PVP) and to elucidate the structure–property relationships governing immobilization efficiency, catalytic activity, and storage stability. Copolymers were synthesized via radical solution polymerization under optimized conditions. Enzymes were immobilized by physical adsorption, and the resulting complexes were characterized by Fourier-transform infrared (FTIR) spectroscopy, protein content assays, proteolytic and amidase activity measurements, and molecular docking. The graft copolymer with a smaller particle size in solution provided a larger accessible surface area, leading to higher bromelain and papain loading. Ficin showed the opposite trend due to its unique surface amino acid composition. Immobilization dramatically increased storage stability: half-life values for bromelain, ficin, and papain reached up to 20, 14, and 14 days, respectively, compared to 1–3 days for the free enzymes. Molecular docking revealed that the dense polymer shell stabilizes the enzyme tertiary structure by forming multiple contacts with internal cavities and tunnels, thereby preventing autolysis and conformational unfolding. Collectively, these findings demonstrate that SA-g-PVP copolymers are promising, non-toxic supports for cysteine proteases, with ficin showing up to 100% activity recovery, making them suitable for food, cosmetic, and biomedical applications. Full article

Background/Objectives: Protein nanocages are versatile platforms with potential applications in drug delivery, enzyme encapsulation, and bioreactor systems, owing to their precise self-assembly and excellent biocompatibility. However, most protein cage systems have limited accessibility to their internal space, which hinders the efficient encapsulation of large molecules or complex proteins. Methods and results: In this study, we propose a programmable reassembly system by artificially splitting the monomer of lumazine synthase, a protein that naturally forms a nanocage through self-assembly. Using intein-mediated protein splicing, the self-assembly of the monomer was converted into a condition-dependent reaction, enabling the incorporation of large or functional biomolecules prior to the assembly stage. Furthermore, to achieve targeted delivery, an EGFR-binding affibody (EGFRAfb) was fused to the split monomer so that it is exposed on the cage surface after reassembly, thereby providing selective binding capability toward EGFR-expressing cells. Successfully reassembled nanocages were visualized, and the fluorescent proteins encapsulated within them were delivered to the target and activated in specific cells. Conclusions: Therefore, the programmable protein nanoplatform presented in this study can overcome the spatial limitations of conventional protein cages while allowing for precise control over both the timing of cage assembly and targeted molecular delivery. Full article

Fresh fish fillets are highly perishable even under refrigerated conditions due to psychrotrophic microbial growth, enzymatic activity, and lipid oxidation. This study evaluated the individual and combined effects of chitosan edible coating and vacuum packaging on the quality and shelf life of Pangasianodon hypophthalmus fillets stored at 4 ± 1 °C for 15 days. Four treatments were applied: uncoated aerobic (U-A), uncoated vacuum (U-V), chitosan-coated aerobic (Ch-A), and chitosan-coated vacuum (Ch-V). Quality changes were assessed through chemical, physical, microbiological, and sensory analyses. Total volatile base nitrogen (TVB-N) increased rapidly in U-A (3.5–22.4 mg N/100 g), whereas lower values were observed in Ch-V (13.3 mg N/100 g). Peroxide value (PV) increased to 1.43 meq O₂/kg fat in U-A but remained lowest in Ch-V (0.77 meq O₂/kg fat). Total plate count (TPC) exceeded the acceptability limit in U-A by day 15, while Ch-V remained within safe limits (6.03 log CFU/g). Coated treatments maintained more stable pH, and chitosan coating reduced moisture loss under aerobic storage. Sensory quality declined rapidly in U-A but was best preserved in Ch-V. The combined application of chitosan coating and vacuum packaging exhibited a clear synergistic effect, extending the refrigerated shelf life of fillets to at least 15 days compared with 9–12 days in uncoated samples. This approach represents an effective and eco-friendly strategy for maintaining the quality and safety of fresh fish products. Full article

Proteins with additives, especially in small quantities, are of great interest as a subject of study. Machine learning approaches implemented on Raman spectroscopy data could provide an insight into the chemical structures of such mixtures or conjugates. Although decision tree models could be powerful in solving either classification or regression tasks and could provide accessible predictions, they are prone to overfitting. Ensemble models that implement several decision trees could overcome the determined problem. Five different model types are discussed: RandomForest, GradientBoosting, AdaBoost, Voting, and Stacking. Raman spectroscopy data of whey protein isolates (5 wt.%) with different amounts of hyaluronic acid (0, 0.1, 0.25, and 0.5 wt.%) were used as datasets. In order to generalize the results of the study, WPI samples from three different manufacturers were used. Optimization established that ensembles of 200 decision trees with a maximum depth of four were optimal. The Stacking algorithm, which used RandomForest, GradientBoosting, and AdaBoost as base models with either LogisticRegressor (classification task) or RidgeCV (regression task), was found to be the most efficient in finding differences between the whey protein isolate and its conjugates with hyaluronic acid: specificity of 68.7% and sensitivity of 95.4% (classification task); R² = 0.764 with mean absolute error of 0.068 (regression task). According to the feature importance plots, the Raman bands that were most influential in predicting the results were 1003 cm⁻¹ (phenylalanine, ring breath), 1125 cm⁻¹ (rocking of NH₃⁺), 1206 cm⁻¹ (C–C stretching), 1240 cm⁻¹ (amide III (β-sheet), N–H in-plane bend, C–N stretch), and 1399 cm⁻¹ (aspartic and glutamic acids, C=O stretch of COO–). The findings of this study may contribute to the development of novel methods for quality control and analysis of complex multicomponent systems in various industrial settings. In particular, the ensemble approach can be adapted for monitoring in food processing or as a screening tool in pharmaceutical formulation development. Full article

Mushrooms have been used for centuries in traditional folk medicine for the treatment of various diseases and are valued for their health-promoting properties. This long-standing use has sparked growing scientific interest in mushrooms as a source of bioactive compounds. While mushrooms contain a wide range of biologically active substances, including terpenoids, alkaloids, and glycoproteins, this review focuses specifically on polysaccharides derived from mushroom and their potential anti-aging effects at the cellular level. The evidence presented here summarizes current knowledge based on both in vitro and in vivo studies. Additionally, this review highlights the emerging potential of mushroom-derived polysaccharides as natural carriers in advanced drug delivery systems. Although several studies have investigated the use of fungal polysaccharides in combination with therapeutic agents—such as bovine serum albumin, resveratrol, paclitaxel, and quercetin—the potential of combining fungal polysaccharides with senotherapeutics remains unexplored. To fully realize the potential of mushroom-derived polysaccharides in promoting everyday health, combating cellular aging and obtaining synergistic anti-ageing effect via using mushroom polysaccharides as carriers for senolytics, further research is needed. Full article

The linear economic model continues to drive multidimensional environmental problems, as it generates large volumes of plastic waste, as well as agricultural by-products, such as coconut husks. On the other hand, the maritime industry still relies on conventional materials such as wood, steel, and fibre-reinforced plastics, which have several usage challenges, including corrosion, toxicity, and difficulties associated with end-of-life management. These issues point to the need for more sustainable material options. This review examines the potential of combining coconut fibre (coir) with recycled plastics to produce a functional material for use in the maritime sector. The material is designed to add value to waste streams by providing a practical approach to reducing dependence on conventional and less sustainable resources. The review discusses fibre treatments (alkali, silane, acetylation) and fabrication methods (compression moulding, extrusion) and evaluates their impact on mechanical performance and durability. The studies show that coir–plastic composites possess highly tuneable mechanical properties. Tensile strengths are reported to range from approximately 2.4 MPa for natural resin matrices to 78 MPa for polyester hybrids, while the flexural modulus can be increased by up to 99% compared to the neat polymer blend. Fibre treatments (e.g., alkali) and fabrication methods are crucial, as they have been shown to improve tensile and flexural strength by over 40% and impact strength by 150%. However, the composites produced still show vulnerability to water absorption, UV radiation, and biofouling, which could limit their application in marine environments. To this end, several issues require further study, including long-term field validation, enhanced understanding of material fatigue, and scalable manufacturing. Full article

Injectable hydrogels have attracted substantial and rapidly growing interest due to their ability to be administered into cavities of any shape and provide local therapeutic treatment. This study reports the synthesis and characterization of thermosensitive microgels and hydrogels obtained via photoinitiated copolymerization of methacrylated gelatin (GN-MA) and N-isopropylacrylamide (NIPAM) in the absence and presence of N,N′-methylenebisacrylamide (MBA). The effects of monomer concentration, crosslinker content (MBA), and irradiation time on product yield, grafted chain length, and material properties were systematically investigated. Depending on the polymerization conditions, microgel samples exhibited hydrodynamic diameters in the range of 354–1022 nm at 20 °C, which decreased to 183–308 nm upon heating to 40 °C. Freeze-drying of the microgel dispersions resulted in the formation of a porous sponge-like structure with pore sizes of 50–90 µm. Rheological studies of the hydrogel properties demonstrated evident thermoresponsive behavior, with storage moduli (G′) ranging from 20 to 600 Pa, matching the mechanics of certain soft tissues. The hydrogels showed high equilibrium swelling capacity at 20 °C, which was reduced at 40 °C, as well as temperature-dependent moxifloxacin release (38–88% over 6 days) and excellent biocompatibility (>85% cell viability) with human skin fibroblasts. These findings make them promising for biomedical applications such as postoperative cavity filling and local drug delivery. Full article

Lignocellulosic agricultural residues are abundant yet underutilized despite their potential for sustainable bioconversion. This study evaluated spent mushroom substrate (SMS) from Pleurotus ostreatus cultivation and roots of leafy vegetables (RLV) as alternative substrates for Pleurotus production, using wheat straw as a control. Two species, P. ostreatus and P. citrinopileatus, were cultivated on different SMS/RLV ratios and the immunomodulatory potential of harvested mushrooms was assessed. Specifically, protein (PE-D-P3 < 3 kDa) and carbohydrate (CE-D) fractions obtained after in vitro digestion were applied to LPS-challenged THP-1 cells and immune-related gene expression was analyzed by qPCR. Both species significantly modulated immune responses. The PE-D-P3 showed a more pronounced immunomodulatory effect, significantly downregulating IL1B, IL6 and TNF, whereas the CE-D reduced only TNF expression. Substrate composition influenced bioactivity: PE-D-P3 from SMS 80-RLV 20% resulted in the greatest reduction in IL1B, IL6 and TNF, while CE-D from SMS 60-RLV 40% reduced IL1B and CXCL8. These findings provide insights that both fungal species and substrate composition influence immunomodulatory compound production. Valorizing lignocellulosic residues through optimized mushroom cultivation represents a sustainable strategy for producing functional ingredients with applications in human and animal health, particularly for preventing inflammation-related disorders. Full article

The increasing prevalence of drug-resistant microorganisms has prompted research into novel antimicrobial compounds, with 2-thiophene carboxylic acid thiourea derivatives showing promise for future therapeutic applications. However, the poor water solubility of these compounds limits their practical use. This study investigates the formation and characterization of inclusion complexes between 2-hydroxypropyl-β-cyclodextrin (HPβCD) and 2-thiophene carboxylic acid-halogenated (chlorine-, bromine-, and iodine-) thiourea derivatives, seeking to improve their physicochemical properties. The dynamic light scattering (DLS) measurements and UV-Vis spectroscopy provided information related to thiourea–HPβCD aggregates and stoichiometry. Solid-state inclusion compounds and physical mixtures were prepared in two different molar ratios (thioureas:HPβCD = 1:1 and 1:2), and the morphology of the resulting powders was observed by scanning electron microscopy (SEM). Thermogravimetry (TG) and differential scanning calorimetry (DSC) (TG-DSC) coupled analysis were used to analyze thermal profiles in the temperature range of 25 °C to 600 °C, while the spectral data obtained by Fourier transform infrared spectroscopy (FTIR) provided the characteristic vibrational bands of the pure guest molecules and data corresponding to the structural and chemical changes in the host–guest systems. The structural and thermal analyses revealed significant interactions between the host and thioureas molecules, with evidence of possible interactions involving two cyclodextrin molecules. The results demonstrate the presence of intermediate stoichiometry in the inclusion compounds, with possible enhancement of the therapeutic potential of these thiourea derivatives. Full article

Polymer-based dressings constitute an important class of macromolecular biomaterials enabling controlled drug delivery and enhanced wound healing performance. This review summarizes recent advances in the design, fabrication, and functionalization of polymer dressings, with emphasis on natural and synthetic polymer systems applied in biomedical topical and transdermal drug administration. Key material properties, including biocompatibility, mechanical stability, porosity, and degradation behavior, are discussed in relation to drug loading capacity and release kinetics. Current fabrication strategies, such as electrospinning, hydrogel formation, casting, and multilayer assembly, are critically evaluated with respect to structural control and scalability. Particular attention is given to antimicrobial and stimuli-responsive platforms capable of dynamic interaction with the wound microenvironment. Furthermore, challenges related to long-term stability, regulatory requirements, and clinical translation are addressed. By integrating recent experimental findings, this review highlights essential structure–function relationships governing polymer dressing performance and provides design guidelines for next-generation macromolecular topical and transdermal care systems with improved multifunctionality and clinical applicability. Full article

The construction sector is responsible for substantial energy consumption, greenhouse gas emissions, and resource depletion, driving the search for sustainable alternatives to conventional petroleum-based insulation materials. Lignocellulosic biomass, comprising cellulose, hemicellulose, and lignin, offers a renewable resource for the development of bio-based foams with potential application in construction systems. This review provides a comprehensive analysis of bio-based foams tailored to building applications, positioning recent scientific advances against the technical properties of commercial synthetic insulation foams. Key performance parameters, including density, thermal conductivity, compressive strength, dimensional stability, water vapour diffusion resistance, and fire behaviour, are critically examined. Developments in lignocellulosic-based foams are discussed, highlighting processing strategies such as crosslinking, chemical modification, and hybrid reinforcement to enhance mechanical, thermal, and fire performance. The reported results demonstrate that lignin-based polyurethane and phenolic foams can achieve competitive compressive strength and thermal insulation, while cellulose-based aerogels and foams exhibit ultra-low density and promising conductivity values. However, challenges related to moisture sensitivity, fire classification, process scalability, standardisation, and market integration remain significant. Overall, lignocellulosic foams represent a promising pathway toward decarbonised, circular construction systems, provided that technical optimisation and regulatory alignment are successfully achieved. Full article

In this work, an in situ UV-assisted photoreduction was used to functionalize silk fibroin films with silver nanoparticles in order to develop antibacterial devices for wound healing applications. The process showed high efficiency (~80%) in terms of reacted silver precursor. The effects of the silver treatment on fibroin macromolecule were evaluated in function of the process parameters in terms of chemical structure, thermal and mechanical properties, swelling behavior, resistance to degradation and antibacterial activity. Silver functionalization significantly improved the mechanical properties of the films, with Young’s modulus increasing from 0.23 ± 0.04 MPa (methanol-treated samples) to 7.26 ± 0.46 MPa (silver-functionalized samples). In parallel, a marked reduction in swelling degree was observed (from ~360–420% to ~60%), indicating enhanced structural stability. The treated films also exhibited improved resistance to degradation over 7 days under physiological conditions. From a functional perspective, the materials showed strong antibacterial activity, with up to 97–98% reduction in bacterial proliferation for Pseudomonas aeruginosa and Escherichia coli, and up to 93% for methicillin-resistant Staphylococcus aureus. Overall, the results demonstrate that silver functionalization process improves the structural stability of silk fibroin while conferring sustained antibacterial activity, thus supporting their potential application as antimicrobial dressings for the treatment of superficial and low-exudate wounds. Full article

This review analyzes the advances over a five-year period in the development of polymeric sorbents for the purification of aqueous media from key classes of pollutants: hydrocarbons (crude oil, diesel fuel), organic dyes, pharmaceuticals (antibiotics), pesticides, herbicides, volatile organic compounds, and polycyclic aromatic hydrocarbons. Attention is paid to the analysis of structure-property-performance relationships, with an emphasis on comparing materials derived from renewable natural feedstocks (such as cellulose, chitosan, terpenes, vegetable oils, and aloe vera) with synthetic polymers. The analysis reveals that biopolymer-based sorbents exhibit comparable or superior sorption capacities combined with environmental safety, biodegradability, and low cost. The key sorption mechanisms include physical adsorption, hydrophobic interactions, and electrostatic interactions. Despite persisting challenges related to scalability, stability in real-world environments, and the need for efficient regeneration protocols, a convergent approach that combines the advantages of modified natural polymers and functional synthetic components appears to be the most promising strategy for developing cost-effective and sustainable technologies for the restoration of water quality. Full article

Fibroin-based films represent a promising platform for sustainable and bio-derived materials. Existing literature has mainly focused on isolated molecules, plasticizers, or chemical cross-linkers, and the function of complex, multi-component natural extracts as structure-modulating agents in fibroin films remains poorly understood. In this study, edible films containing mulberry leaf extract (MLE; 2–8 wt%) and fibroin (8 wt%) were prepared by solution casting, and their structures were investigated using spectroscopic, morphological, thermal, mechanical, and barrier property analyses. The results reveal that MLE induces concentration-dependent changes in film performance through multicomponent, non-covalent interactions with the fibroin. An approximately 187% increase in tensile strength was achieved at high MLE concentration, confirming effective physical reinforcement. The water vapor transmission rate decreased markedly from 0.888 to 0.170 g·h⁻¹·m⁻², indicating an enhanced moisture barrier, whereas oxygen permeability increased at higher extract loadings, suggesting localized chain rearrangements. High optical transparency in the visible region was maintained (79.95–83.77%), while UV response was selectively altered with extract concentration. Overall, the 8MLE formulation exhibited the most balanced performance. This study demonstrates that plant-derived extracts can serve as effective natural modifiers for tailoring fibroin film properties without inducing crystallization, offering a sustainable strategy for designing bio-based and edible protein film systems. Full article

This study focuses on the development and characterization of advanced composite materials based on poly(ε-caprolactone) (PCL) and poly(vinylidene fluoride) (PVDF), with or without silver nanoparticles (AgNPs), planned for peripheral nerve or bone regeneration. The complementary properties of PCL (biocompatibility and biodegradability) and PVDF (mechanical stability and piezoelectric functionality) were exploited by blending the polymers in different ratios, resulting in binary (PCL/PVDF) and ternary (PCL/PVDF/AgNPs) composites. Green-synthesized AgNPs were integrated to enhance antimicrobial activity and to support tissue repair through improved signal transmission. Functional thin films and electrospun fibres were obtained and subjected to advanced characterization techniques, including scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), and thermal analysis. The results demonstrated appropriate morphology, chemical composition, structural stability, and favourable interactions with simulated physiological media. Preliminary biocompatibility assays confirmed good cell viability, supporting the biomedical applicability of the designed scaffolds. Overall, the obtained results highlight the potential of AgNPs-functionalized PCL/PVDF binary and ternary composites as promising candidates for flexible, durable, and bioactive implants in peripheral nerve or bone regeneration. Full article

This study developed poly(lactic acid) (PLA) biocomposites reinforced with pine wood flour (10, 20, and 30 wt%) to achieve the interphase through chemical modification. Specifically, the wood flour was treated with poly(propylene glycol) toluene 2,4-diisocyanate terminated (PEGTDI), while 1 wt% poly(lactic acid)-g-maleic anhydride (PLA-g-MA) was integrated as a reactive compatibilizer during extrusion and thermocompression. Fourier-transform infrared spectroscopy (FTIR) analysis corroborated the occurrence of urethane formation and ester/anhydride linkages, as substantiated by the presence of characteristic bands indicative of surface carbamation at 1645 and 1726 cm⁻¹. Thermal analysis revealed that both the pine wood flour and coupling agents promoted PLA crystallization; however, thermogravimetric analysis (TGA) indicated a decrease in thermal stability for functionalized composites, suggesting a trade-off between enhanced interfacial interaction and heat resistance. Mechanical testing demonstrated a significant reinforcement effect, with the Young’s modulus increasing by up to 22% in untreated composites. The coupling agents effectively optimized stress transfer at low fiber loadings (10 wt%), while flexural modulus improvements were predominant at higher loadings (20–30 wt%) regardless of treatment. These findings underscore the criticality of surface modification and compatibilizer selection for tailoring the structural and thermo-mechanical properties of PLA-based biocomposites, thereby providing a pathway for optimized performance in structural applications. Full article