Heterogeneous nanostructured materials are currently studied as promising electrode materials for lithium-ion batteries (LIBs) due to effective synergy. Herein, we report on TiO2-B@VS2 heterogeneous nanowire arrays (TVNAs) as additives-free anodes for LIBs. The VS2 is a two-dimensional (2D) material with intrinsically metallic nature. Importantly, this layered 2D material offers a large interlayer spacing for facile intercalation of lithium-ions and possesses a high theoretical capacity. The TVNAs electrode shows a reversible capacity of 365.4 mA h g−1 after 500 cycles at a current density of 1 C (335 mA g−1), being significantly superior than the pure TiO2-B nanowire arrays (TNAs) electrode (192.7 mA h g−1). Impressively, the TVNAs electrode delivers a high rate capacity of 171.2 mA h g−1 at 10 C rate. The merits of the TVNAs electrode could be ascribed to the outstanding structural stability of the TNAs and the high capacity and conductivity of VS2.