Gel Electrolytes With Regulated Ion Channels and Stabilized Zn Interfaces Enable Durable Flexible Zinc–Air Batteries

ABSTRACT Flexible zinc–air batteries require gel electrolytes that simultaneously reconcile rapid ion transport, mechanical robustness, and stable Zn interfacial chemistry. Here, a trehalose‐regulated L‐PAT/PVA gel electrolyte is developed through hierarchical bulk–interface regulation. Hofmeister‐induced PVA crystallization provides a mechanically reinforced framework, while trehalose‐mediated competitive hydrogen bonding moderates excessive chain association, reconstructs the local hydration environment, and preserves continuous low‐tortuosity ion‐transport pathways. Simultaneously, sulfonate groups from L‐carrageenan regulate the Zn/electrolyte interfacial microenvironment, homogenize local ionic flux, and direct Zn electrocrystallization toward the (002)‐preferred orientation. DRT analysis further reveals suppressed slow‐polarization contributions and more stable interfacial kinetics during cycling. The optimized electrolyte exhibits a tensile strength of 609 kPa, a fracture strain above 1200%, and an ionic conductivity of 154.5 mS cm −1 . The resulting flexible Zn–air battery delivers 77 mW cm −2 peak power density, ≈200 mAh cm −3 volumetric capacity, and stable cycling for 250 h at 1 mA cm −2 , while maintaining reliable operation from −15 C to 55°C and under mechanical deformation.