Conventional hydrogels face fundamental challenges in reconciling sensing adaptability with on-demand protection for emerging intelligent wearables. Inspired by the stress-induced hardening mechanism of sea cucumbers, we have developed an innovative thermoresponsive composite hydrogel that overcomes these limitations through carefully engineered multicomponent integration. The outstanding performance arises from dynamically crosslinked poly(acrylic acid)-amorphous calcium carbonate coordination networks, which serve as thermally responsive phase-transition elements. Additionally, hierarchically structured cellulose nanofiber/carbon nanotube (CNT/CNF) percolation networks provide both mechanical reinforcement and electrical conductivity, creating synergistic interactions between these components. The resulting hydrogel demonstrates exceptional thermoresponsive behavior with a remarkable 826-fold increase in compressive modulus. Beyond this dramatic mechanical transition, the material integrates multiple advanced functionalities, including autonomous fast self-healing within 1s, moldable shaping, good electrical conductivity, and extreme stretchability beyond 1000 % strain. This unique combination of properties facilitates a novel dual-mode operation, where the material serves simultaneously as a highly sensitive strain sensor for continuous physiological monitoring and as an adaptive protective system capable of rapid electrothermal-triggered stiffening in less than 3 s. When implemented in protective device architectures, the system demonstrates a 45.58-fold increase in bending strength upon activation, from 0.19 MPa to 8.66 MPa, along with exceptional impact energy absorption of 30.87 kJ m−2. These capabilities represent a significant breakthrough in adaptive material design, establishing a new paradigm for smart systems that seamlessly integrate real-time sensing with active protection.
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