Surface-modified carbon nanoparticles (CNPs) as reinforcement materials have attracted significant attention due to their potential for substantially enhancing mechanical properties. However, the development and application of CNP-enhanced polymeric materials are constrained by an incomplete understanding of their reinforcement mechanisms, impeding sustainable progress. In this study, we employed molecular dynamics simulations to investigate the mechanical properties of surface-modified CNP-reinforced epoxy resin composites at the microscopic scale. The simulations focused on the tensile process and the nanopinning effect of CNPs within the epoxy resin matrix. Our results indicate that surface-modified CNPs form stronger interfacial connections with the epoxy resin, leading to enhanced mechanical strength of the composites. Quantitative analysis revealed that these composites exhibit higher tensile strength compared to nonmodified counterparts, with a significant improvement in stability due to the robust noncovalent interactions between CNPs and the epoxy matrix. This study elucidates the reinforcement mechanisms of surface-modified CNPs in polymers, providing valuable insights for further optimization and sustainable development of CNP-reinforced polymeric materials.