Lithium　(Li)　has　garnered　considerable　attention　as　an　alternative　anodes　of　next-generation　high-performance　batteries　owing　to　its　prominent　theoretical　specific　capacity.　However,　the　commercialization　of　Li　metal　anodes　(LMAs)　is　significantly　compromised　by　non-uniform　Li　deposition　and　inferior　electrolyte–anode　interfaces,　particularly　at　high　currents　and　capacities.　Herein,　a　hierarchical　three-dimentional　structure　with　CoSe2-nanoparticle-anchored　nitrogen-doped　carbon　nanoflake　arrays　is　developed　on　a　carbon　fiber　cloth　(CoSe2–NC@CFC)　to　regulate　the　Li　nucleation/plating　process　and　stabilize　the　electrolyte–anode　interface.　Owing　to　the　enhanced　lithiophilicity　endowed　by　CoSe2–NC,　in　situ-formed　Li2Se　and　Co　nanoparticles　during　initial　Li　nucleation,　and　large　void　space,　CoSe2–NC@CFC　can　induce　homogeneous　Li　nucleation/plating,　optimize　the　solid　electrolyte　interface,　and　mitigate　volume　change.　Consequently,　the　CoSe2–NC@CFC　can　accommodate　Li　with　a　high　areal　capacity　of　up　to　40 mAh cm–2.　Moreover,　the　Li/CoSe2–NC@CFC　anodes　possess　outstanding　cycling　stability　and　lifespan　in　symmetric　cells,　particularly　under　ultrahigh　currents　and　capacities　(1600　h　at　10 mA cm−2/10 mAh cm−2　and　5 mA cm−2/20 mAh cm−2).　The　Li/CoSe2–NC@CFC//LiFePO4　full　cell　delivers　impressive　long-term　performance　and　favorable　flexibility.　The　developed　CoSe2–NC@CFC　provides　insights　into　the　development　of　advanced　Li　hosts　for　flexible　and　stable　LMAs.　©　2022　The　Authors.　Advanced　Science　published　by　Wiley-VCH　GmbH.