The　practical　application　of　lithium　(Li)　metal　anode　has　been　greatly　hampered　by　irregular　growth　of　Li　dendrites　and　the　volume　expansion　during　the　cycle.　Constructing　a　three-dimensional　lithiophilic　porous　framework　is　regarded　as　an　effective　solution.　Here,　using　a　CuO　nanocluster　arrays–decorated　carbon　fiber　cloth　(CuO-NC@CFC)　to　prestore　Li　via　molten　infusion　has　been　testified　to　effectively　resolve　these　bottlenecks.　Impressively,　after　a　violent　melt-infusion　process,　the　constructed　nanostructures　can　be　maintained　and　transformed　into　Cu/Li2O　nanocluster　arrays,　together　with　highly　conductive　carbon　fiber　cloth,　provide　fast　charge　transport　during　Li　stripping/plating　process.　As　demonstrated　by　finite　element　simulations　and　experimental　evidence,　the　formed　Cu/Li2O　nanocluster　arrays　not　only　redistribute　Li+　flux　and　reduce　local　current　density　but　also　serve　as　Li　nucleation　sites.　Consequently,　the　as-acquired　Li/Cu-NC@CFC　electrodes　could　significantly　buffer　volume　fluctuation　and　regulate　Li　deposition　behavior,　exhibiting　an　ultrastable　and　ultralong　lifespan　(400　h　at　5　mA/cm2　with　1　mAh/cm2　Li　and　800　h　at　5　mA/cm2　with　5　mAh/cm2　Li　in　symmetric　cells).　When　coupled　with　LiFePO4,　the　Li/Cu-NC@CFC　electrode　could　deliver　a　high　capacity　of　110.3　mAh/g　after　500　cycles　at　2　C.　©　2021　Elsevier　Ltd