Hydrogen Bond Enhanced Multifunctional Hydrogel Enabling Fibrous Zn‐Ion Battery‐Integrated Sensing System

Achieving compact flexible energy storage battery‐sensor integration device is crucial for constructing future portable and multifunctional wearable electronics, which enables intelligent sensing, battery status self‐monitoring, and human‐machine interactions. Here, a multifunctional tamarind polysaccharide/chitosan (PTC) hydrogel combining good mechanical properties and high ionic conductivity was fabricated by introducing multiscale hydrogen bonds into a polyacrylamide network. Thus, this multifunctional hydrogel fiber exhibits enhanced sensing sensitivity and improved gel‐electrolyte properties, enabling seamless energy storage‐sensor integration. As a result, the fibrous device delivers a long‐term stable power supply, highly sensitive external stimulus detection, and constant battery status self‐monitoring. The fibrous battery well retains 87.34 % capacity after repeated bending to 120° and 200 cycles, while the fibrous sensor exhibits high sensitivity (gauge factor = 207.57) with a broad detection range (0 %–700 %). The battery‐integrated sensing system also enables real‐time monitoring of motion and realizes human‐machine interaction, offering an effective pathway to integrate high‐sensitivity sensing with stable energy storage.