Unlocking Anode‐Free Zinc Metal Batteries via Data‐Science‐Guided Dual‐Interphase Separator Engineering

ABSTRACT Aqueous zinc metal batteries (AZMBs) employing halogen‐ or manganese‐based cathodes and anode‐free design possess the highest energy density among the aqueous battery families. However, their performance is severely limited by interfacial side reactions and anode‐cathode cross‐talk, which undermine energy density and cycle life. Conventional strategies focusing on a single interface are inadequate to address these systemic issues. The optimal strategy cluster from literature data mining guided the material system creation via a data‐driven process of molecular descriptor screening. This guided the creation of an asymmetric dual‐interphase separator, featuring a Zn 2+ ‐supplying interphase (ZSI) on the anode side that suppresses polyhalide shuttling and accelerates desolvation, and a composite conductive interphase (CCI) on the cathode side that enhances multi‐electron reaction kinetics and active species utilization. Enabled by the asymmetric dual‐interphase engineering, the constructed anode‐free Zn||MnO 2 full cell achieves a high voltage efficiency of 90% and stable cycling over 1000 cycles. Concurrently, a state‐of‐the‐art anode‐free Zn||I 2 battery delivers an energy efficiency exceeding 90% at high areal loading of 38.14 mg cm −2 . Furthermore, a universal zinc metal anode/electrolyte interphase descriptor (ZMAEID) was proposed, mechanistically linking interfacial electrochemical behavior with mechanical stability. This systematic, data‐driven, and theory‐guided strategy establishes a new paradigm for next‐generation anode‐free AZMBs.