TiO2-graphene nanocomposite was first synthesized by a facile gas/liquid interface reaction. The structure and morphology were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and Brunauer–Emmett–Teller measurements. The results indicate that TiO2 nanoparticles (ca. 10nm in mean grain size) were successfully deposited onto the graphene sheets during the gas/liquid interfacial reaction process. The electrochemical performance was evaluated by using coin-type cells versus metallic lithium in an enlarged potential window of 0.01–3.0V. A high specific charge capacity of 499mAhg−1 was obtained at a current density of 100mAg−1. More strikingly, the TiO2-graphene nanocomposite exhibits excellent rate capability, even at a high current density of 3000mAg−1, the specific charge capacity was still as high as 150mAhg−1. The high specific charge capacities can be attributed to the facts that graphene possesses high electronic conductivity, and the lithium storage performance of graphene is delivered during discharge/charge processes of TiO2-graphene nanocomposite between 0.01 and 3.0V.