Si Yu Zheng, Afei Liu, Xianhui Zhang, Wenhui Wu, Lihui Chen, Chunmei Lai, Yuekun Lai, Kai Liu
Abstract Most hydrogels rely heavily on cryoprotectants to enhance their anti‐freezing capabilities; however, this approach is often accompanied by disadvantages such as altered network structures and the risk of cryoprotectant leakage in aqueous conditions. Given these challenges, an environmentally resilient diode‐like hydrogel is developed, featuring a double‐layer coating design inspired by the physiological characteristics of penguins. This design is achieved through plasma treatment and immersion in 3‐aminopropyltriethoxysilane/butyl acetate and perfluoropolyether carboxylic acid/butyl acetate solutions, constructing a double‐layer coating with stable interfacial strength. The coating not only enhances anti‐dehydration performance but also imparts anti‐freezing properties via N,N‐dimethylformamide solution. By carefully regulating the coating thickness and polymerization duration, it has optimized the mechanical and electrical attributes of hydrogel, culminating in robust performance even at −80 °C. The hydrogel exhibits exceptional water retention capabilities, with a mere 33.4% water loss rate following 7 days of air drying. Moreover, the hydrogel demonstrates stable piezoionic output performance across various low‐temperature environments, with tensile and compressive strengths of 1156 kPa and 3.45 MPa, respectively. This study presents a novel solution for the application of conductive hydrogels in smart wearable devices, underscoring their potential for use in extreme environments.