Muscle-Fiber-Inspired Solid-State Ionic Conductive Elastomers with High Strength, Toughness, and Self-Healing Capability

Solid-state ionic conductors mitigate issues such as solvent evaporation and liquid leakage inherent in gel-based systems. However, achieving a synergistic combination of integrated performance properties─including excellent mechanical strength, high ionic conductivity, efficient self-healing capability, and long-term stability─remains a pressing challenge. Here, inspired by the architecture of muscle fibers, this work designed a dual network comprising dynamic boroxine covalent cross-links and a supramolecular network formed by acylsemicarbazide (ASC) hydrogen bonds. The resulting polyurethane-based solid-state ion-conductive elastomer (PUIL 0.3 ) demonstrated exceptional integrated performance, achieving a tensile strength of 38.10 MPa, a toughness of 289.42 MJ m –3, and a high ionic conductivity of 3.06 × 10 –5 S cm –1 . Additionally, PUIL 0.3 exhibits efficient self-healing performance, excellent tear resistance, recyclability, and long-term stability. The sensor fabricated from PUIL 0.3 achieves a high sensitivity (Gauge Factor = 6.58) over an ultrabroad strain range (0.1%–1000%). Moreover, PUIL 0.3 has been successfully applied in human motion monitoring and mechanical energy harvesting, demonstrating its potential as a multifunctional flexible device. Inspired by muscle fibers, the covalent–supramolecular dual-network strategy proposed in this study offers a universal and efficient approach for simultaneously enhancing the mechanical properties, conductivity, and environmental stability of polymer-based solid-state ionic conductors.