Dragonfly Wing‐Inspired Reticular Hierarchical Structure Enables Strong and Tough Supramolecular Elastomers

Abstract Dragonfly wings possess exceptionally high strength, toughness, and fatigue resistance due to their unique hierarchical structure from the micro to macro scale. Inspired by this, mismatched supramolecular interactions (MMSIs) are introduced into the dynamic acylsemicarbazide groups, constructing an interconnected hybrid network of soft and hard segments in the SPUU‐DS elastomer. This design, featuring a dense array of hydrogen bonds, achieves exceptional mechanical properties: a true stress at breaks of 1.1 GPa comparable to that of typical spider silk (0.8–1.5 GPa); toughness of 325.54 MJ m ⁻³ , twice that of typical spider silk (≈160 MJ m ⁻³ ); and a fracture energy of 232.83 kJ m ⁻² , surpassing many metals and alloys. Furthermore, a monitoring device with a “hamburger” structure is developed by integrating SPUU‐DS with a conductive graphene film. When placed inside a tire, this device enhances the tire's puncture resistance by approximately twofold. By correlating the resistance signals with puncture angles, the system enables the detection of damage at various locations on the tire, allowing for timely repair of damage and preventing traffic accidents. This novel biomimetic approach, inspired by dragonfly wings, provides valuable insights for designing healable elastomers with superior mechanical properties.