From Bonds to Barriers: Amphiphilic Molecules Enable Dual Interfacial and Electrolyte Regulation for Highly Stable Aqueous Zinc‐Ion Batteries

ABSTRACT The uncontrolled growth of zinc dendrites and severe parasitic side reactions critically impede the practical development of aqueous zinc‐ion batteries (AZIBs), largely due to the high activity of water molecules in aqueous electrolytes. Herein, we report arbutin (HQOGP) as a green and multifunctional electrolyte additive capable of simultaneously stabilizing the electrolyte and zinc anode interface. Comprehensive experimental investigations combined with theoretical calculations reveal that the hydrophilic glucose moiety of HQOGP reconstructs the hydrogen‐bonding network of the electrolyte, suppressing water activity and the hydrogen evolution reaction. Concurrently, the zincophilic hydroquinone group preferentially adsorbs onto the zinc surface, directing Zn 2+ deposition along the thermodynamically favorable Zn(101) crystal plane and enabling uniform, compact, and dendrite‐free zinc growth. Benefiting from these synergistic effects, the Zn//Zn symmetric cell achieves stable cycling for 800 h at 10 mA cm −2 , while the Zn//Cu half‐cell delivers highly reversible cycling over 1600 cycles at 1 mA cm − 2 . Furthermore, the Zn//VO 2 full cell retains 87.73% of its initial capacity after 2000 cycles at 5 A g − 1 . This work demonstrates an effective strategy for concurrently mitigating dendrite formation and water‐induced side reactions through rational electrolyte design for durable aqueous metal batteries.