An Ultrahighly Stretchable and Recyclable Starch‐Based Gel with Multiple Functions

Abstract With the development of various gel‐based flexible sensors, novel gels with multiple integrated and efficient properties, particularly recyclability, have been developed. Herein, a starch‐based ADM (amylopectin (AP)–poly(3‐[dimethyl‐[2‐(2‐methylprop‐2‐ enoyloxy)ethyl]azaniumyl]propane‐1‐sulfonate) (PDMAPS)–MXene) gel is prepared by a facile “cooking” strategy accompanying the gelatinization of AP and polymerization reaction of zwitterionic monomers. Reversible crosslinking in the gel occurs through hydrogen bonding and electrostatic interactions. The ADM gel exhibits high stretchability (≈2700%, after one month), swift self‐healing performance, self‐adhesive properties, favorable freezing resistance, and satisfactory moisturizing properties (≥30 days). Interestingly, the ADM gel can be recycled and reused by a “kneading” method and “dissolution–dialysis” process, respectively. Furthermore, the ADM gel can be assembled as a strain sensor with a broad working strain range (≈800%) and quick response time (response time 211 ms and recovery time 253 ms, under 10% strain) to detect various macro‐ and micro‐human‐motions, even under harsh conditions such as pronunciation and handwriting. The ADM gel can also be used as a humidity sensor to investigate humidity and human respiratory status, suggesting its practical application in personal health management. This study provides a novel strategy for the preparation of high‐performance recycled gels and flexible sensors.