Graphene-Based Coating Strategies to Realize High Performance Cementitious Composites: A Perspective from Carbon-Neutrality

Graphene-based nanosheets (GNS), including graphene, graphene oxide (GO), reduced graphene oxide (rGO), and graphene nanoplatelets (GNPs), have attracted increasing attention for developing high-performance and sustainable cementitious composites. Compared with conventional dispersion strategies, graphene-based coating strategies enable the targeted localization of GNS at critical interfacial transition zones (ITZs), thereby maximizing their reinforcing efficiency while mitigating agglomeration issues. This review systematically summarizes recent advances in GNS coating technologies for cementitious composites, including physical adsorption, chemical assembly, electrophoretic deposition, and in situ growth. The effects of GNS coatings on interfacial engineering, mechanical performance, durability enhancement, and smart functionalities are critically discussed. Existing studies indicate that GNS coatings can improve strength, crack resistance, impermeability, and resistance to chloride ingress, freeze–thaw cycles, and other degradation processes mainly through ITZ densification and microstructure refinement. However, these benefits are strongly dependent on the coating method, substrate type, and stability of the graphene–substrate interface in calcium-rich alkaline pore solutions. In particular, physically adsorbed GO coatings may suffer from desorption or Ca²⁺-induced aggregation, chemically assembled coatings require further validation beyond laboratory-scale systems, and electrophoretic deposition is mainly applicable to electrically conductive substrates. In addition, localized conductive networks created by GNS coatings facilitate multifunctional properties such as self-sensing, electromagnetic shielding, and electrothermal performance. From a carbon-neutrality perspective, the improvements in mechanical properties and durability provide opportunities to reduce material consumption, extend service life, and lower life-cycle carbon emissions. Nevertheless, their carbon-neutral contribution should be verified through quantitative life-cycle assessment rather than inferred directly from strength or durability enhancement alone. Finally, the remaining challenges associated with large-scale implementation, long-term stability, cost-effectiveness, and field-scale validation are discussed. Particular attention is given to the fact that most existing evidence is derived from laboratory-scale specimens rather than real structural elements exposed to service environments.