CuS and Cu1.8S have been investigated respectively as anodes of lithium-ion batteries because of their abundant resources, no environment pollution, good electrical conductivity, and a stable discharge voltage plateau. In this work, CuS/Cu1.8S nanocomposites were firstly prepared simultaneously by the one-pot synthesis method at a relatively higher reaction temperature 200 °C. The CuS/Cu1.8S nanocomposites anodes exhibited a high initial discharge capacity, an excellent reversible rate capability, and remarkable cycle stability at a high current density, which could be due to the nano-size of the CuS/Cu1.8S nanocomposites and the assistance of Cu1.8S. The high electrochemical performance of the CuS/Cu1.8S nanocomposites indicated that the CuxS nanomaterials will be a potential lithium-ion battery anode.