Yuanyuan Yang, Chao Tan, Dan Zhang, Hengbo Jia, Ziyi Cheng, Qian Li, An Liu, Guotai Sun, Zhifeng Deng, Hengwei Qiu, Yongqiang Ji, Le Li
ABSTRACT To solve the interface challenge, an electrolytic derivative zinc oxide (EZO) protective layer rich in surface hydroxyl groups and oxygen vacancies was constructed, and on this basis, a coordinated “hydrogen‐bond passivation and defect‐guided regulation” interface regulation mechanism was established. In this framework, the surface hydroxyl groups reorganized the interface water environment through competitive hydrogen bond interaction, effectively regulated water activity, and promoted the gradual dissolution of Zn 2+ ions. At the same time, the intrinsic oxygen vacancies acted as electron‐rich anchor positioning points to guide the transport of desolvated Zn 2+ and promote uniform 2D nucleation and transverse growth during zinc deposition. Due to this optimized interface reaction pathway, EZO@Zn anodes provided highly reversible electrochemical behavior in various cathodic chemistries, including iodine, manganese, and vanadium‐based systems. Consequently, under the high current density of 10 A g −1 , the corresponding full cell showed a capacity retention rate of 97 % after 10 000 cycles, while maintaining fast interface mass transport and charge transfer kinetics within a wide temperature window of −10°C to 45°C. In addition to the coin cell configuration, the assembled pouch cell could continuously power micro drones, highlighting the practical feasibility of this interface strategy in multi‐system integration and real‐world energy storage applications.