Bio‐Inspired Highly Stretchable and Ultrafast Autonomous Self‐Healing Supramolecular Hydrogel for Multifunctional Durable Self‐Powered Wearable Devices

Abstract As skin bioelectronics advances, hydrogel wearable devices have broadened perspectives in environment sensing and health monitoring. However, their application is severely hampered by poor mechanical and self‐healing properties, environmental sensitivity, and limited sensory functions. Herein, inspired by the hierarchical structure and unique cross‐linking mechanism of hagfish slime, a self‐powered supramolecular hydrogel is hereby reported, featuring high stretchability (>2800% strain), ultrafast autonomous self‐healing capabilities (electrical healing time: 0.3 s), high self‐adhesiveness (adhesion strength: 6.92 kPa), injectability, ease of shaping, antimicrobial properties, and biocompatibility. It is observed that by embedding with the highly hygroscopic salt LiCl in supramolecular hydrogel, the hydrogel not only showed excellent electrical conductivity but also presented favorable anti‐freezing and water retention properties in extremely cold environments and natural settings. Given these attributes, the hydrogel served as a multifunctional durable self‐powered wearable device with high sensitivity (gauge factor: 3.68), fast response time (160 ms), low detection limit, and frequency sensitivity. Moreover, the multifunctional applicability of this supramolecular hydrogel is further demonstrated in long‐term cold environments sensing, remote medical communication, and underwater communication. Overall, these findings pave the way for the sustainable development of hydrogel‐based wearable devices that are self‐powered, durable, and offer high performance, environmental adaptability, and multi‐sensory capabilities.