Stress‐Triggered Ionic Rearrangement Produces Self‐Strengthening Eutectogels With Decoupled Mechanical Rigidity and Ionic Conductivity

ABSTRACT High‐performance conductive gels possess exceptional mechanical robustness yet exhibit compromised ductility, conductivity, and self‐reinforcement capability, owing to the impeded ion transport and restricted dynamic reconstruction within dense networks. This dilemma is overcome here by a stress‐triggered ionic rearrangement strategy that exploits the dynamic reorganization of mobile ions to decouple ionic conductivity from structural rigidity. This strategy engineers a network saturated with dispersed free ions to guarantee superior conductivity independent of structural density, triggers in situ aggregation of these ions into high‐density ionic cross‐linking domains upon deformation, and consequently activates a potent self‐strengthening mechanism that reaches a maximum of 185% of the initial value. Consequently, this structural evolution translates into an unprecedented convergence of mechanical robustness and functional agility, yielding a tensile strength of 34.58 MPa, an elastic modulus of 77.38 MPa, and a volumetric toughness of 177.3 MJ/m 3 . Crucially, such extreme mechanical reinforcement is achieved without compromising the dynamic nature, preserving a high extensibility of 644.5% alongside efficient ionic conductivity. Leveraging this unique material platform, we develop a flexible sensor with a detection limit of 10 µm. The sensor demonstrates precise recognition of diverse physiological activities, from large‐scale limb movements to subtle signals such as swallowing, pulse, and respiration.