In this manuscript, we utilize a facile and efficient step-by-step strategy to synthesize three-layered C@TiO2@MoS2 hierarchical nanocomposites. These novel hybrids serve as anode materials in lithium-ion batteries (LIBs). The designed structure, in which MoS2 nanosheets are uniformly grown on TiO2 coated carbon hollow spheres, can enhance the electrical conductivity of electrodes, shorten the diffusion length of Li+ ions, alleviate the expansion of electrode materials and provide more active sites for lithium ion storage. As anode materials for lithium-ion batteries (LIBs), the C@TiO2@MoS2 hierarchical nanocomposites exhibit a high initial specific capacity (1687 mA h g-1) and good cycling performance (993.2 mA h g-1 after 100 cycles at a current density of 0.2 A g-1). Furthermore, the C@TiO2@MoS2 electrode exhibits high rate capacities of 963, 860, 806, 743, 703, 664 and 633 mA h g-1 at different current densities of 200, 500, 1000, 2000, 3000, 4000 and 5000 mA h g-1, respectively. The electrochemical performances stated above prove that the as-prepared C@TiO2@MoS2 nanocomposites can be promising anode materials for high-performance lithium-ion batteries.