Rapid Self‐Healing and Self‐Adhesive Supramolecular‐Polymer Double‐Network Eutectogels for Wearable Flexible Sensors in Human‐Machine Interaction

ABSTRACT The development of gel‐based soft materials has greatly promoted the advancement of flexible electronic devices. However, fabricating gels with excellent overall properties for dynamic, complex environments remains challenging. Herein, we report a supramolecular‐polymer double‐network (SP‐DN) eutectogel constructed in a deep eutectic solvent (DES) using natural folic acid (FA) supramolecules and a betaine‐based zwitterionic polymer, poly [2‐(methacryloyloxy)ethyl]diethy‐(3‐sulopropyl) (PMAEDS). The incorporation of the FA supramolecular network endows the FA/PMAEDS SP‐DN eutectogel with remarkable rapid self‐healing capability (within 10 s), while significantly enhancing its mechanical strength and ionic conductivity. Moreover, the eutectogel exhibits broad temperature tolerance and strong self‐adhesiveness. Benefiting from these synergistic features, the FA/PMAEDS SP‐DN eutectogel serves as an efficient wearable sensing material. The sensor demonstrates high sensitivity (gauge factor, GF = 4.32) and a fast response time (200 ms), enabling real‐time monitoring of diverse human motions. When applied to key body regions, this sensor further facilitates the remote operation of robotic arms, highlighting its great potential for next‐generation human‐machine interaction interfaces.