Hydrogen Bond‐Engineered Dual‐Phase Cellulose‐Polyelectrolyte Ionogel for All‐Weather Health Monitoring and Human‐Machine Interaction

ABSTRACT Cellulose ionogels are highly attractive for next‐generation wearable and flexible electronics, sensing, and energy storage applications. However, synchronously enhancing mechanical and electronic performance without compromising environmental stability remains a significant challenge. Here, cellulose ionogels with controllable phase separation (RCPAA) are fabricated via hydrogen‐bonding regulation, wherein the polyelectrolyte‐derived dual‐phase structure enables the synergistic optimization. Consequently, RCPAA simultaneously achieves high ionic conductivity and superior mechanical properties, while maintaining long‐term mechanical stability and ion‐leakage‐free performance from −18°C to 100°C. Moreover, RCPAA exhibits reliable sensing performance and adhesion, allowing for multi‐site human motion monitoring and physiological health monitoring. By integrating machine learning and gesture recognition algorithms, an intelligent gesture control system and wearable human‐machine interaction electronics are constructed. The dual‐phase design strategy imparts robust mechanical and electrical properties, providing a promising foundation for broad applications in wearable electronics, intelligent human‐machine interaction, and digital inheritance of traditional arts.