Stimulation‐Reinforced Cellulose–Protein Ionogels with Superior Mechanical Strength and Temperature Resistance

Ionogels, recognized for their flexibility and ionic conductivity, show considerable promise across various applications including electronic skins, biomedical electronics, and smart robotics. However, the majority of ionogels are plagued by suboptimal mechanical strength, a restricted range of operating temperatures, and poor recyclability. Here, an acetone‐stimulated supramolecular reinforcement strategy to develop robust and environmentally tolerant ionogels is introduced. The bio‐based ionogels feature a firm supramolecular architecture formed by the entwining of soybean protein molecules around cellulose macromolecular chains. This coiled design, inspired by cucumber vines, endows the ionogels with remarkable tensile strength (>30 MPa), enables them to withstand temperature above 85 °C with tensile strength over 15 MPa, and maintains notable cold resistance down to −20 °C with tensile strength exceeding 10 MPa. Further, the bio‐based ionogels exhibit excellent recyclability, reprocessing capabilities, shape customizability, good biocompatibility, and full biodegradability. This study provides a valuable strategy for manipulating supramolecular conformation to create robust ionogels that overcome the traditional trade‐offs of high strength and environmental tolerance. A cellulose–protein ionogel, featuring robust mechanical strength and temperature resistance, is developed via supramolecular stimulation. This synthesized ionogel demonstrates exceptional mechanical properties, with a strength exceeding 30 MPa, and can withstand temperatures above 150 °C. In addition, it offers excellent recyclability and processability, showing significant potential for applications in e‐skin and sustainable bioplastics.