Abstract
ABSTRACT
Aqueous zinc‐ion batteries (AZIBs) offer a path to safe and sustainable energy storage, yet their practicality is hindered by subzero failure, parasitic hydrogen evolution, and interfacial degradation. A key challenge is that preserving water mobility at low temperatures can inadvertently promote parasitic hydrogen evolution under ambient conditions. Here, we design a hydrogel electrolyte that combines a wide operating‐temperature window with enhanced interfacial stability through coupled thermodynamic–kinetic regulation of the electrolyte environment. By disrupting the tetrahedral hydrogen‐bond network and diversifying local coordination environments, the hydrogel enhances configurational disorder and suppresses water crystallization. Simultaneously, restricted molecular dynamics retard ice nucleation and parasitic hydrogen evolution. This hydrogen‐bond architecture further promotes rapid and uniform Zn deposition by regulating the thermodynamics and kineticsof interfacial Zn
2+
transfer. Consequently, AZIBs achieve exceptional stability: over 8000 h in symmetric cells, 15 000 cycles in full cells, and high reversibility down to −30°C. This work establishes thermodynamic–kinetic coupling as a promising strategy for designing high‐performance aqueous batteries under extreme conditions.