Here stretchable, self‐healable, and transparent gas sensors based on salt‐infiltrated hydrogels for high‐performance NO2 sensing in both anaerobic environment and air at room temperature, are reported. The salt‐infiltrated hydrogel displays high sensitivity to NO2 (119.9%/ppm), short response and recovery time (29.8 and 41.0 s, respectively), good linearity, low theoretical limit of detection (LOD) of 86 ppt, high selectivity, stability, and conductivity. A new gas sensing mechanism based on redox reactions occurring at the electrode–hydrogel interface is proposed to understand the sensing behaviors. The gas sensing performance of hydrogel is greatly improved by incorporating calcium chloride (CaCl2) in the hydrogel via a facile salt‐infiltration strategy, leading to a higher sensitivity (2.32 times) and much lower LOD (0.06 times). Notably, both the gas sensing ability, conductivity, and mechanical deformability of hydrogels are readily self‐healable after cutting off and reconnection. Such large deformations as 100% strain do not deprive the gas sensing capability, but rather shorten the response and recovery time significantly. The CaCl2‐infiltrated hydrogel shows excellent selectivity of NO2, with good immunity to the interference gases. These results indicate that the salt‐infiltrated hydrogel has great potential for wearable electronics equipped with gas sensing capability in both anaerobic and aerobic environments.

Smart sensing fabrics are becoming increasingly attractive in the emerging wearable areas of medical and military so far. Here, for the first time, we present a smart humidity sensing fabric (SHSF) based on a moisture‐sensitive polyacrylamide hydrogel for respiratory monitoring and non‐contact sensing. Fabricated by in situ cross‐linking of the hydrogel precursors on the fibers of the fabric, the flexible SHSF shows excellent sensitivity, outstanding flame retardance, air permeability, water retention capacity, and stability after treatment with lithium bromide solution. Specifically, its conductance increases more than 311 times as humidity increased from 11% to 98%. Besides, the humidity sensor features good repeatability and the ability to work normally under folding due to its flexible nature. As a clothing material, hydrogel–fabric composite exhibits 4.3 times the burning time compared to cotton fabric, illustrating better flame retardance. The SHSF is used to monitor human breathing and non‐contact finger approaching in real time, demonstrating its flexibility in practical applications. This work provides strategies for preparing high‐performance, flame‐retardant SHSF for emerging wearable electronic devices.