Dual‐Mixing High‐Entropy Strategy Via Cation and Solvent Co‐Engineering for Wide‐Temperature Aqueous Zinc‐Ion Batteries

Abstract Aqueous zinc‐ion batteries hold great promise for safe and sustainable energy storage, but their practical deployment is severely hindered under extreme temperatures by electrolyte freezing, intensified corrosion, and hydrogen evolution. Herein, we propose a dual‐mixing high‐entropy strategy that simultaneously introduces multiple cations (Zn 2+ , Mg 2+ , Ca 2+ , and Li + ) and organic solvents (dimethyl sulfoxide and acetone) into a ZnCl 2 ‐based aqueous electrolyte. This synergistic design significantly amplifies configurational entropy, effectively disrupting the hydrogen‐bond network and suppressing ice nucleation, achieving an extremely low glass transition temperature of −105°C without detectable crystallization. The highly disordered solvation structure reduces water activity, suppresses parasitic side reactions, and stabilizes the zinc–electrolyte interface, enabling highly uniform and dendrite‐suppressed zinc deposition. Consequently, the dual‐mixing electrolyte enables stable symmetric cell cycling for over 1400 h at −40°C and 1600 h at 30°C. Zn||polyaniline full cells deliver over 1000 cycles across −40°C to 50°C, retaining 72% capacity even at 50°C. This work demonstrates that dual‐mixing high‐entropy design is a promising strategy for all‐climate aqueous zinc‐ion batteries.