The nanocrystalline CoSb2 was prepared by a solvothermal method at various temperatures and was investigated as a potential anode material for lithium-ion batteries. It was found that the CoSb2 is highly crystallized at 190°C and with almost a single-phase structure. The morphology of the alloy powder plays an important role in their cycling behavior. The large reversible capacity and better capacity retention of these nanosized CoSb2 alloys make them promising anode materials for Li-ion batteries.