High　performance　lithium　metal　anode　is　of　great　importance　to　achieve　batteries　with　high　energy　density.　Due　to　the　intrinsic　high　reactivity　of　Li　metal　anode　and　the　insufficient　understanding　of　lithium　redox　at　the　Li/electrolyte　interface,　the　fast　and　dendrite-free　Li　metal　deposition　still　remains　a　grand　challenge.　In　this　work,　we　accelerate　Li+/Li　redox　through　the　regulation　of　the　electric　double　layer　(EDL),　in　which　2-Mercaptopyridine　(2-MP),　a　conjugated　weak-base　molecule　with　stable　electrochemical　properties,　can　be　specifically　adsorbed　on　Li　metal　surface　and　promote　charge　transfer.　It　fundamentally　avoided　the　formation　of　Li　metal　dendrites　and　enabled　fast　Li　plating/stripping　process,　leading　to　uniform　Li　deposition　as　well　as　superior　cycling　performances　of　batteries.　This　work　provides　a　significant　contribution　to　the　understanding　of　battery　chemistry　at　the　electrode/electrolyte　interface.　©　2023　Elsevier　B.V.