Balancing Interfacial Adsorption and Ion Migration Through a High‐Entropy‐Engineered Oxide for Durable Zinc Anodes

ABSTRACT Oxide coatings, owing to their electronic insulation and ionic conductivity, are promising artificial interfacial layers for stabilizing Zn anodes. However, conventional single‐phase, multiphase, and low‐entropy oxides remain insufficient to simultaneously address the complicated interfacial challenges in aqueous zinc‐ion batteries. Herein, inspired by high‐entropy engineering, an ultrathin amorphous high‐entropy‐engineered oxide TiYZrAlSnO x (TYZAS) coating is in situ constructed on Zn anodes via atomic layer deposition to achieve durable interfacial stabilization. Beyond the conventional perception that strong zincophilicity is universally beneficial, a lever‐like thermodynamic–kinetic balance between Zn adsorption and ion migration is revealed, demonstrating that insulating oxide coatings favor weak yet effective Zn adsorption coupled with rapid Zn 2+ migration. Both experimental and theoretical results demonstrate that the TYZAS coating simultaneously reduces Zn adsorption strength and migration barrier, thereby promoting homogeneous Zn nucleation and accelerated interfacial ion transport. Consequently, the TYZAS‐protected Zn anode delivers an ultralong cycling lifespan of 4000 h at 5 mA cm −2 and 1 mAh cm −2 . This work establishes a generalizable interfacial thermodynamic–kinetic regulation principle for the rational design of advanced Zn metal anodes.