The　performance　of　zinc-ion　batteries　is　severely　hindered　by　the　uncontrolled　growth　of　dendrites　and　the　severe　side　reactions　on　the　zinc　anode　interface.　To　address　these　challenges,　a　weak-water-coordination　electrolyte　is　realized　in　a　peptone-ZnSO4-based　electrolyte　to　simultaneously　regulate　the　solvation　structure　and　the　interfacial　environment.　The　peptone　molecules　have　stronger　interaction　with　Zn2+　ions　than　with　water　molecules,　making　them　more　prone　to　coordinate　with　Zn2+　ions　and　then　reducing　the　active　water　in　the　solvated　sheath.　Meantime,　the　peptone　molecules　selectively　adsorb　on　the　Zn　metal　surface,　and　then　are　reduced　to　form　a　stable　solid-electrolyte　interface　layer　that　can　facilitate　uniform　and　dense　Zn　deposition　to　inhabit　the　dendritic　growth.　Consequently,　the　Zn||Zn　symmetric　cell　can　exhibit　exceptional　cycling　performance　over　3200 h　at　1.0 mA cm−2/1.0 mAh cm−2　in　the　peptone-ZnSO4-based　electrolyte.　Moreover,　when　coupled　with　a　Na2V6O16·3H2O　cathode,　the　cell　exhibits　a　long　lifespan　of　3000　cycles　and　maintains　a　high　capacity　retention　rate　of　84.3%　at　5.0 A g−1.　This　study　presents　an　effective　approach　for　enabling　simultaneous　regulation　of　the　solvation　structure　and　interfacial　environment　to　design　a　highly　reversible　Zn　anode.　©　2023　Wiley-VCH　GmbH.