Regulating Hydrogen Bond Competition to Break Ultrawide‐Temperature (−70°C to 100°C) Limits for All‐Climate Zinc Batteries

ABSTRACT Hydrogel electrolytes endow aqueous zinc‐metal batteries with inherent safety and mechanical flexibility, rendering them compelling for wearable energy storage. However, their narrow operating temperature range and poor rate capability remain critical bottlenecks. In this study, a hydrogen‐bond (HB) regulation strategy based on a multifunctional hydrogel electrolyte (PAM‐NAEL, composed of Zn(ClO 4 ) 2 , polyacrylamide (PAM), and N‐acetyl‐L‐glutamine (NAEL)) is proposed to exploit the physicochemical nature of HBs, thereby improving both the operational temperature window and rate performance. Specifically, the NAEL component dynamically reshapes the internal HB network by competing for HB sites. This reconfiguration suppresses ice nucleation at low temperatures and maintains structural integrity at high temperatures, enabling an ultrawide temperature tolerance. Furthermore, the dynamic network lowers the ion migration barrier and accelerates deposition kinetics, endowing the advanced Zn||Zn symmetric cells with an ultrawide temperature adaptability (−70°C to 100°C) and outstanding rate capability (1 to 40 mA cm −2 ). Notably, even at an extremely low temperature of −40°C, the cells maintain exceptional cyclability exceeding 7500 h. Additionally, the Zn||I 2 full‐cell can operate stably over 10000 cycles at −20°C. Remarkably, the practical Zn||I 2 pouch cell with high mass‐loading I 2 cathode (10.60 mg cm −2 ) and limited N/P ratio (2.8) retains 95.12% capacity after 400 cycles.