A one-step hydrothermal process was employed to prepare a series of MoS2 nanostructures via simply altering the surfactant as soft template and hydrothermal reaction temperature. Three kinds of MoS2 nanostructures (three-dimensional (3D) hierarchical nanospheres, one-dimensional (1D) nanoribbons, and large aggregated nanoparticles) were successfully achieved and investigated well by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), high resolution transmission electron microscopy (HRTEM), and Brunauer–Emmett–Teller analysis (BET). Electrochemical tests reveal that these MoS2 samples could deliver high initial discharge capacities (higher than 1050.0mAhg−1), but various cycling performances. The hierarchical MoS2 nanospheres assembled by sheet-like subunits show the highest specific capacity of 1355.1mAhg−1, and 66.8% of which can be retained after 50cycles. The good lithium storage property of hierarchical MoS2 nanospheres can be attributed to the higher electrolyte/MoS2 contact area and stable 3D layered structure.