LAUSR

Hydrogels have entered the spotlight for applications in soft electronics. It is essential and challenging to obtain hydrogels that can function properly under varying environmental circumstances, that is, 30–90% relative humidity (RH) and −20 to 40 °C due to their intrinsic nature to lose and absorb water upon variations in humidity and temperature. In this work, a green solvent, solketal, is introduced into poly 3‐dimethyl‐2‐(2‐methylprop‐2‐enoyloxy)ethyl azaniumyl propane‐1‐sulfonate (poly(DMAPS)) zwitterionic hydrogels. Compared to glycerol, solketal endows hydrogels with greater possibility for further modification as well as improved water content and mechanical performance consistency over 30–90% RH. Encouragingly, the optimized hydrogel demonstrates its unique merits as a dielectric layer in iontronic sensors, featuring non‐leaky ions, high sensitivity (1100 kPa−1), wide humidity, and temperature range applicability. A wide‐humidity range healable and stretchable electrode is attained by combining the hydrogel substrate with Ag paste. A full‐device healable and highly‐sensitive sensor is developed. This study is a pioneering work that tackles the broad humidity range applicability issue of hydrogels, and demonstrates the ion‐leakage‐free ionic skins with zwitterionic dielectrics. The outcomes of the study will considerably promote advancements in the fields of hydrogel electronics and iontronic sensors.