▎ 摘　　要

Unfilled rubbers usually show poor mechanical properties. Here, we demonstrate toughening natural rubber (NR) by designing a compact hybrid filler network composed of graphene (GE) and carbon nanotubes (CNTs). The physical interactions in this network have a bond energy lower than covalent bonds; and thus they preferentially break upon deformation and serve as sacrificial bonds that dissipate energy before failure of the materials. The high energy dissipation of the hybrid filler network not only increases the fracture toughness and tensile strength, but also suppresses the crack growth of the NR/GE/CNT nanocomposites. These properties will provide the nanocomposites with better sustainability during practical applications.