In this report, three-dimensional hierarchically structured aerogels constructed with ultrathin layered MoS2/graphene nanosheets (3DMG) synthesized with a facile one-pot hydrothermal method, are employed as anodes for lithium-ion batteries (LIBs) without conductive additives, polymer binders or metal current-collectors. Due to the integration of three-dimensional porous structure and ultrathin layered MoS2/graphene, the 3DMG aerogel anode exhibits a high reversible capacity and an excellent high-rate capability. In addition, the 3DMG aerogels anode maintains a capacity of ∼870mAhg−1 at 1Ag−1 after 200 cycles, demonstrating superior long-cycle performances of 3DMG aerogels at a high current density. The reported 3DMG aerogels have promising application potentials in highly-efficient lightweight LIBs.