Highly Sensitive, Degradable, and Rapid Self‐Healing Hydrogel Sensor with Semi‐Interpenetrating Network for Recognition of Micro‐Expressions

Abstract Flexible conductive hydrogels have revolutionized the lives and are widely applied in health monitoring and wearable electronics as a new generation of sensing materials. However, the inherent low mechanical strength, sensitivity, and lack of rapid self‐healing capacity results in their short life, poor detection accuracy, and environmental pollution. Inspired by the molecular structure of bone and its chemical characteristics, a novel fully physically cross‐linked conductive hydrogel is fabricated by the introduction of nanohydroxyapatite (HAp) as the dynamic junction points. In detail, the dynamically cross‐linked network, including multiple physical interactions, provides it with rapid self‐healing ability and excellent mechanical properties (elongation at break (>1200%), tensile strength (174kPa), and resilience (92.61%)). Besides, the ions (Cl − , Li + , Ca 2+ ) that move freely within the system impart outstanding electrical conductivity (2.46 ± 0.15 S m −1 ), high sensitivity (gauge factor, GF>8), good antifreeze (−40.2 °C), and humidity properties. The assembled sensor can be employed to sensitively detect various large human motions and subtle changes in behavior (facial expressions, speech recognition). Meanwhile, the hydrogel sensor can also degrade in phosphate‐buffered saline solution without causing any environmental pollution. Therefore, the designed hydrogels may become a promising candidate material in the future potential applications for smart wearable sensors and electronic skin.