Elastic Yet Strength Triboelectric Aerogel Enabled by Constructing a Supramolecular System

Abstract Elastic aerogels are ultra‐lightweight, highly porous materials widely used in fields such as sensing, aerospace, and thermal insulation. However, constrained by weak mechanical properties under deformation, the strength and elasticity of aerogels are mutually exclusive and difficult to reconcile. In this study, a triboelectric aerogel with a centripetal structure is constructed using a supramolecular system in combination with ice‐templating, resulting in outstanding mechanical properties (specific strength of 186.67 kN m kg −1 ) and rapid recovery speed (792 mm s −1 ). The key to reconciling strength and elasticity lies in multiscale structural synergy, mitigating local stress through controlled inelastic deformation to balance resistance and deformation. A portable triboelectric sensor is developed based on this material, offering motion protection and posture monitoring. This study addresses the challenge of reconciling elasticity and strength in aerogels, providing new insights for designing elastic smart materials.