Aluminum　metal　with　high　capacity　has　been　regarded　as　a　promising　anode　material　for　lithium　ion　batteries　but　suffers　from　pulverization　and　side　reactions　upon　the　lithiation　and　de-lithiation　process,　which　depend　on　the　rational　design　and　controllable　synthesis　of　nanostructures.　Here,　it　is　proposed　that　ultrathin　aluminum　nanosheets　(Al-NS)　grown　on　carbon　nanotubes　as　anode　materials　for　lithium　ion　batteries.　Based　on　the　preferential　Al(111)　crystal　facet　exposure　and　the　rather　limited　thickness　less　than　5　nm,　the　batteries　exhibit　a　high　reversible　capacity　of　990　mAh　g−1　at　1　C　and　an　excellent　rate　capacity　of　524.6　mAh　g−1　at　24　C,　and　a　long　term　stability　with　almost　no　capacity　fading　after　500　cycles　at　high　C-rates　of　5,　10,　and　20　C.　Density　functional　theory　based　first　principle　calculation　reveals　that　the　high　Young＇s　modulus　of　Al(111)　facet　for　fast　Li+　diffusion　and　composite　materials　design　with　carbon　nanotubes　enable　high　rate　capability　and　mitigate　huge　volume　change　during　discharge/charge　process.　The　results　prove　that　ultrathin　Al　nanosheets　can　be　a　low　cost　and　high-performance　anode　material　for　lithium　ion　batteries.　©　2021　Wiley-VCH　GmbH.