Multiscale simulations of carbon nanomaterials–reinforced cementitious composites: Mechanical and durability performance

Carbon nanofiller-reinforced cementitious composites (CNRCCs) have been widely investigated due to their potential to enhance mechanical properties, crack resistance, and durability, offering a promising pathway toward resilient and durable infrastructure. However, CNRCCs are predominantly driven by empirical trial-and-error experimentation. This approach is inherently costly and time-consuming, limiting the ability to fully elucidate complex physicochemical mechanisms and achieve optimal design. Multiscale simulation offers a principled pathway to overcome this bottleneck by resolving interactions across length scales, thereby enabling inverse design strategies that enhance performance and reduce costs. In the context of computational modelling efforts using molecular dynamics, micromechanics, and finite element methods (FEM), a critical review that holistically integrates mechanical properties and durability aspects is lacking. This review provides a systematic and critical synthesis on the computational modelling of CNRCCs, covering molecular dynamics (MD), micromechanical modelling, FEM, and emerging data-driven approaches. By linking atomistic interfacial chemistry to structural-scale response, the review shows that surface functionalization markedly improves nanofiller–matrix interactions. Carbon nanotubes (CNTs) can increase interfacial bonding energy by up to 109% and surface fracture energy by 135% compared with pristine CNTs. At the structural scale, FEM studies indicate that a 2 vol% CNT addition can increase critical load capacity by up to 80%, while interfacial shear-strength optimization may increase toughness by over 1900%. Furthermore, this study elucidates the governing mechanisms of durability, including the regulation of ionic transport, carbonation, and nanoconfined water phase transitions. This review provides a rational foundation for the predictive, multiscale-informed design of durable, resilient, and sustainable CNRCCs.