Bioinspired Solvation‐Interfacial Dual Regulation for Subzero‐Tolerant and Long‐Cycling Aqueous Zinc Metal Batteries

ABSTRACT Aqueous zinc metal batteries (AZMBs) hold great promise for large‐scale green energy storage but suffer from Zn‐metal instability caused by dendrite growth, hydrogen evolution, and corrosion. In this work, we introduce inosine (Ino), a natural biomolecule, as an electrolyte additive to address these challenges by leveraging its dual functions of Zn 2+ chelation and Zn‐metal adsorption. Ino effectively replaces water molecules within Zn 2+ solvation sheaths through strong coordination bonds and disrupts the hydrogen‐bonding network among water molecules, thereby reducing free water activity. Simultaneously, Ino preferentially adsorbs onto Zn metal, constructing a stable interfacial layer that guides uniform Zn 2+ deposition. As a result, Zn//Zn symmetric cells exhibit exceptional cycling stability (3300 h) and durability at low temperature (1500 h). Zn//Cu half‐cells achieve a high average Coulombic efficiency of 99.07% over 1000 cycles. Full‐cells paired with NH 4 V 4 O 10 (NVO) cathodes retain 77.9% capacity after 2000 cycles at 5 A g −1 . Furthermore, a Zn//NVO pouch cell with a low negative/positive capacity (N/P) ratio (3.53) retains 79.1% of its initial capacity after 290 cycles. A more practical pouch cell delivers an initial capacity of 61.14 mAh and maintains stable operation for 100 cycles, underscoring its real‐world viability. This biomolecule‐derived solvation‐interfacial dual‐regulation strategy provides a novel approach for designing eco‐friendly, high‐performance AZMBs.