He Zhang, Weibin Jia, Mingze Sun, Yuxiang Chen, Xiaoyi Zhang, Hao Li, Xingdao He, Peng Shi, Lizhi Xu
Ionogels are promising for soft robotics, energy systems, and bioelectronic interfaces due to their high ionic conductivity and environmental stability. However, combining high strength and fracture resistance remains challenging. Here, we report composite ionogels with outstanding mechanical strength (~65.4 megapascal) and fracture energy (~607 kilojoules per square meter), capable of bearing more than 5000 times their own weight. These ionogels are developed by tailoring solvent-solute interactions to create a dense, hyperconnected nanofibrous polymer network. Solvent engineering regulates hydrogen bonding competition, facilitating the formation of robust interphase hydrogen bonds and a soft-hard biomimetic interface. Moreover, their antidrying, breathable nature enables multifunctional electrophysiological monitoring, making them ideal for wearable bioelectronics. Their ionic conductivity, drug-loading capacity, and antibacterial properties allow their use in advanced e-bandages for chronic wound healing. This generalizable strategy for ionogel design opens pathways toward strong, versatile, and biocompatible materials, particularly valuable for next-generation soft materials, wearable electronics, and tissue engineering.