Won Seok Lee

We showcase self‐oscillating gel systems exhibiting an expanded operating temperature and accompanying functional adaptability. The developed system contains nonthermoresponsive main‐monomers, such as N,N ‐dimethylacrylamide (DMAAm) or 2‐acrylamido‐2‐methylpropane sulfonic acid (AMPS) or acrylamide (AAm) or 3‐(methacryloylamino)propyl trimethylammonium chloride (MAPTAC). The gels volumetrically self‐oscillates within the range of the conventional (20.0 °C) and extended (27.0 and 36.5 °C) temperatures. Moreover, the gels successfully adapt to the environmental changes; they beat faster and smaller as the temperature increases. The period and amplitude are also controlled by tuning the amount of main‐monomers and N ‐(3‐aminopropyl) acrylamide. Furthermore, the record amplitude in the bulk gel system consisting of polymer strand and crosslinker at 36.5 °C is achieved (≈ 10.8%). Our study shows new self‐oscillation systems composed of unprecedented combinations of materials, giving the community a robust material‐based insight for developing more life‐like autonomous biomimetic soft robots with various operating temperatures and beyond. This article is protected by copyright. All rights reserved