The　carbonic　current　collector　of　graphene-assembled　film　(GF)　is　fabricated　at　scale　by　a　roll-to-roll　process　to　improve　the　performance　of　lithium-ion　batteries.　The　obtained　GF　current　collector　possesses　large　crystallites　(61.18　nm),　a　high　degree　of　three-dimensional　(3D)　ordering　(90.6%　AB　Bernal　stacking),　and　good　interlayer　alignments,　thereby　demonstrating　outstanding　lightweight　(1.57　mg　cm-2),　excellent　thermal　conductivity　(1531.7　W　m-1　K-1),　high　electrical　conductivity　(1.09　×　106　S　m-1),　excellent　flexibility　(30　000　times　bending),　and　flame　retardancy.　By　substituting　the　Al　current　collector　with　GF　in　cells,　the　LiFePO4　cathode　realizes　a　50.7%　increase　of　the　specific　energy　by　lightening　the　mass　of　inactive　components.　The　cells　equipped　with　GF　current　collector　can　also　obviously　enhance　the　rate　and　cycling　abilities　by　reducing　the　interfacial　contact　resistance　and　rapidly　dissipating　heat　generated　during　charging/discharging　at　a　high　current　density.　This　novel　strategy　for　the　scalable　fabrication　of　an　ultralightweight　GF　current　collector　possesses　great　potential　for　practical　application　by　offering　more　reliable　cells　with　better　rate　capability　and　specific　energy.　©　2023　American　Chemical　Society.