MoS2/C nanocomposite with a multilayered sandwich structure based on few-layered MoS2 and carbon layers in an alternating sequence, was successfully synthesized through a one-step synchronized carbonization and sulfuration method. The hybrids were characterized by X-ray diffraction, High-resolution transmission electron microscopy, Atomic force microscope, Raman and X-ray photoelectron spectroscopic methods. The as-obtained MoS2/C nanocomposite applied as lithium-ion batteries anode materials, showed a high initial discharge and charge capacities of 1678.5 and 1386.0mAhg−1, respectively. High specific reversible capacity is maintained at fast C rates, e.g., 1390, 1223, 1017, 566, and 450mAhg−1 at 0.1C, 0.6C, 3C, 10C and 20C, respectively. The good performance of the composite is mainly attributed to the unique few layered composite architectures, which can improve ion/electron transportation and prevent aggregation and restacking during the lithiation/delithiation process.