Constructing High‐Performance Composite Epoxy Resins: Interfacial π‐π Stacking Interactions‐Driven Physical Rolling Behavior of Silica Microspheres

Abstract The intrinsic compromise between strength and toughness in composite epoxy resins significantly constrains their practical applications. In this study, a novel strategy is introduced, leveraging interfacial π‐π stacking interactions to induce the “rolling behavior” of microsphere fillers, thereby facilitating efficient energy dissipation. This approach is corroborated through theoretical simulations and experimental validation. The resulting composite epoxy resin demonstrates an impressive 49.8% enhancement in strength and a remarkable 358.9% improvement in toughness compared to conventional epoxy resins, accompanied by substantially reduced hysteresis. Moreover, this system achieves reversible closed‐loop recyclability and rapid repair capabilities. The preliminary demonstration of “force‐temperature equivalence” further establishes a novel pathway for the design of high‐performance composite epoxy materials.