Three-dimensional (3D) nanoarchitectures can improve the performance of electrical energy storage systems. In this paper, combining an improved solvothermal method with calcination treatment, thin layer carbon-coated MoO2 nanoparticles with the size of 20-50nm were uniformly dispersed in 3D graphene aerogel (abbreviated as MoO2@C-Gas). The hybrid materials were subsequently used as a new-structured anode for lithium-ion batteries (LIBs), yielding high reversible capacity with excellent stable cyclability. We found that the battery with MoO2@C-Gas electrode could deliver a discharge capacity of 1515mAhg−1 at a current density of 80mAg−1 in the first cycle, and remain at 1113mAhg−1 over 60 cycles. Furthermore, with the increase of current density, it also exhibited a high rate of capability and good cycling performance. The outstanding performance of the hybrid electrode were attributed to the unique 3D aerogel morphology and the close combination between C@MoO2 and graphene layers, which could significantly improve the anode's electronic conductivity.