Large-scale　application　of　low-cost,　high-safety　and　environment-compatible　aqueous　Zn　metal　batteries　(ZMBs)　is　hindered　by　Zn　dendrite　failure　and　side　reactions.　Herein,　highly　reversible　ZMBs　are　obtained　by　addition　of　trace　D-pantothenate　calcium　additives　to　engineer　a　dual-functional　interfacial　layer,　which　is　enabled　by　a　bioinspired　gating　effect　for　excluding　competitive　free　water　near　Zn　surface　due　to　the　trapping　and　immobilization　of　water　by　hydroxyl　groups,　and　guiding　target　Zn2+　transport　across　interface　through　carboxyl　groups　of　pantothenate　anions,　as　well　as　a　dynamic　electrostatic　shielding　effect　around　Zn　protuberances　from　Ca2+　cations　to　ensure　uniform　Zn2+　deposition.　In　consequence,　interfacial　side　reactions　are　perfectly　inhibited　owing　to　reduced　water　molecules　reaching　Zn　surface,　and　the　uniform　and　compact　deposition　of　Zn2+　is　achieved　due　to　promoted　Zn2+　transport　and　deposition　kinetics.　The　ultra-stable　symmetric　cells　with　beyond　9000 h　at　0.5 mA cm−2　with　0.5 mAh cm−2　and　over　5000 h　at　5 mA cm−2　with　1 mAh cm−2,　and　an　average　Coulombic　efficiency　of　99.8%　at　1 mA cm−2　with　1 mAh cm−2,　are　amazingly　realized.　The　regulated-electrolyte　demonstrates　high　compatibility　with　verified　cathodes　for　stable　full　cells.　This　work　opens　a　brand-new　pathway　to　regulate　Zn/electrolyte　interface　to　promise　reversible　ZMBs.　©　2024　Wiley-VCH　GmbH.