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

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.