A synergistic interfacial and topological strategy for reinforcing aramid nanofiber films.

While nanomaterials possess impressive mechanical properties at the microscale level, their macroscopic assemblies usually exhibit inferior properties due to ineffective stress transfer among individual nanomaterials. This issue is addressed in this work by achieving strong interfacial interactions between aramid nanofibers and graphene oxide nanosheets through a neutralization reaction in a dipolar solvent and regulating the topological properties using polymer micelles to form a compact structure, leading to the formation of a super-strong and super-tough nanofiber film. The film was prepared through a sol-gel-film transition process and possesses a nacre-like microstructure that deflects microcracks and prevents them from propagating straight through the film. Remarkably, it demonstrates a tensile strength of 599.0 MPa and a toughness of 37.7 MJ m, which are 491.0% and 1094.5% that of a pristine aramid nanofiber film, respectively. In addition, it exhibits excellent tolerance to extreme temperatures (-196 to 300 °C) and fatigue resistance to folding 10 000 times. Overall, this study presents a synergistic interfacial and topological enhancement strategy for constructing nanomaterial-based composites with inherited properties from the nanoscale building blocks to the macroscale structural material.