Xiao Huang, Taisong Pan, Taiqi Hu, Runming Zeng, Siqi Chen, Jiaqi Wang, Yang Xiao, Bo Zhao, Bao Zhang, Wei Sun, Yuan Lin
ABSTRACT Flexible aqueous zinc‐iodine batteries (AZIBs) have emerged as promising candidates for the power source in wearable electronics, owing to their intrinsic safety and cost‐effectiveness. However, electrochemical and mechanical interface instability between zinc anodes and electrolytes under deformation prevent the reliable performance of AZIBs in practical applications. Here, we present a synergistic supramolecular interactions engineering strategy utilizing hydrogen bonding, ion‐dipole, and coordination interactions to enhance interfacial stability by creating a polyacrylamide‐trehalose‐ dimethylglycine (PATT) hydrogel electrolyte with strengthened interfacial adhesion, reduced water activity, and facilitated ion transport. With PATT, Zn||ZnI 2 cell delivers an areal capacity of 4.2 mAh cm − 2 with 85.2% retention after 6000 h, while multilayer pouch cell maintains 1.2 Ah with 92.3% retention over 175 cycles. Excellent mechanical resilience and electrochemical stability of Zn||ZnI 2 cells are further observed under successive loading cycles of bending and stretching. The strain‐sensing capability of PATT hydrogel is also investigated, thereby enabling the energy supply and hand motion capture with monolithic material. A smart glove for virtual reality interaction is demonstrated to highlight the potential of PATT hydrogel in achieving mechanical‐robust wearable electronics.