Side　reactions　and　dendrite　growth　triggered　by　the　unstable　interface　and　inhomogeneous　deposition　have　become　the　biggest　obstacle　to　the　commercialization　for　lithium　metal　batteries.　In　this　study,　a　highly-chlorinated　organic-inorganic　hybrid　interfacial　protective　layer　is　developed　by　rationally　tuning　the　interfacial　passivation　and　robustness　to　achieve　the　convenient　and　efficient　Li　metal　anode.　The　polyvinyl　chloride　(PVC)　can　effectively　resist　water　and　oxygen,　which　is　confirmed　by　density　functional　theory.　The　organic-dominant　solid　electrolyte　interphases　(SEI)　with　lithium　chloride　are　investigated　by　the　X-ray　photoelectron　spectroscopy　(XPS)　with　little　mineralization　of　oxide,　such　as　Li2　O　and　Li2　CO3　.　With　such　artificial　SEI,　a　uniform　and　dense　lithium　deposition　morphology　are　formed　and　an　ultra-long　stable　cycle　of　over　500　h　are　achieved　even　at　an　ultra-high　current　density　of　10　mA/cm2　.　Moreover,　the　simple　and　convenient　protected　anode　also　exhibits　excellent　battery　stability　when　paired　with　the　LiNi0.8　Co0.1　Mn0.1　O2　(NCM811)　and　LiFePO4　(LFP)　cathode,　showing　great　potential　for　the　commercial　application　of　lithium　metal　batteries.　(c)　2024　Published　by　Elsevier　B.V.　on　behalf　of　Chinese　Chemical　Society　and　Institute　of　Materia　Medica,　Chinese　Academy　of　Medical　Sciences.