The　development　of　lithium-metal　batteries　(LMBs)　is　seriously　restricted　by　the　out-of-control　dendrites　growth　and　infinite　volume　expansion.　Herein,　a　pervasive　organic-inorganic　layer　construction　strategy　is　reported　for　the　composite　lithium　metal　anode　with　congener-derived　organic-inorganic　solid　electrolyte　interphase　(SEI).　In　this　strategy,　the　organic-inorganic　Ag@polydopamine　(Ag@PDA)　layer　is　coated　on　the　arbitrary　substrates　by　a　simple　two-step　method.　The　thin　and　stable　congener-derived　SEI　is　in-situ　formed　with　fewer　inorganic　components　and　more　organic　components　during　charging/discharging.　The　polydopamine　with　sufficient　adhesion　groups　and　lithiophilic　Ag　layer　realize　near-zero　nucleation　overpotential　during　lithium　deposition.　The　low　interface　resistance　and　stable　lithium　deposition　are　achieved.　Moreover,　the　practical　areal　and　volumetric　capacities　of　the　composite　anode　with　three-dimensional　copper　(3DCu)　as　the　substrate　are　10　mAh/cm2　and　1538　mAh/cm3　(vs.　the　mass　of　anode).　The　symmetrical　cell　shows　very　low　polarization　voltage　(10　mV)　and　more　than　2500　h　cycles　life　at　1　mA/cm2　(1　mAh/cm2).　The　LiNi0.8Co0.1Mn0.1O2　(NCM811)-based　full　cells　show　improved　capacity　retention　(82%)　after　100　cycles　at　0.5　C.　The　modified　lithiophilic　anode　with　congener-derived　interphase　provides　a　promising　strategy　to　realize　the　next-generation　dendrite-free　LMBs.　©　2024