Rational　design　of　advanced　electrode　materials　is　extremely　important　for　high-performance　lithium-ion　batteries　(LIBs).　Herein,　we　report　a　facile　one-pot　hydrothermal　approach　for　formation　of　MoS2/nitrogen-doped　graphene　(MoS2/N-graphene)　composite　with　excellent　lithium　storage　properties　as　anode　for　LIBs.　The　controlled　experiment　results　indicate　that　polyethyleneimine　(PEI)　functionalizes　not　only　as　the　nitrogen　source　for　in-situ　nitrogen　doping,　but　also　as　a　binder　for　inducing　and　regulating　the　uniform　growth　of　MoS2　nanosheets　onto　graphene.　As　a　result,　ultrathin　MoS2　nanosheets　are　vertically　grown　onto　the　nitrogen-doped　reduced　oxide　graphene　(RGO),　generating　a　distinct　honeycomb-like　hybrid　structure.　More　significantly,　the　first　principles　theoretical　calculations　results　manifest　that　there　is　a　strong　interaction　at　the　interface　of　MoS2　and　nitrogen-doped　graphene,　thus　boosting　the　charge　transfer.　The　constructing　MoS2/N-graphene　architecture　demonstrates　the　improved　electrochemical　performances　for　reversible　lithium　storage.　It　shows　a　high　reversible　capacity　of　1025.1　mAh/g　at　a　current　density　of　100　mA/g　and　the　superior　rate　capability,　which　is　mainly　attributed　to　the　pseudocapacitance　contributions.