Super Weather‐Resistant and Self‐Healing Eutectogels via Dynamic Interactions for Wide‐Range Healthcare and Highly Adaptive Human–Machine Interfaces

Abstract To overcome fundamental limitations in flexible sensing, particularly under extreme environments, including subzero temperatures and arid conditions, a weather‐resistant and self‐healing polyvinyl alcohol‐based eutectogel (PN4) is developed through molecular engineering of dynamic bond networks. The material system integrates a zinc trifluoromethanesulfonate/ N ‐methylacetamide/water deep eutectic solvent (DES) platform, which optimizes the solvation structure and reconfigures hydrogen‐bonding architectures, endowing PN4 with cryogenic tolerance (freezing point < –80 °C) and dehydration (83.8% mass retention over 30 days). Benefiting from dynamic hydrogen bonds and borate ester bonds, PN4 demonstrates strong interfacial adhesion (13.2 kPa to paper), ultrafast self‐healing (healing duration <0.65 s), and high stretchability (371.5% breaking elongation). When configured as a sensor, PN4 exhibits low contact resistance (10.4 kΩ at 1 kHz), rapid response (0.265 s), and durable cycling (200 cycles). As a proof‐of‐concept, this PN4‐based sensor system captures high‐fidelity physiological signals encompassing electrocardiograms, electromyograms, electroencephalograms, and electrooculograms. Furthermore, this system enables an intelligent gesture‐recognition platform operational at −20 °C. This versatility and robustness highlight the broad prospects of eutectogels in portable/wearable electronics in challenging environments.