A simple method is developed for the preparation of MoSe2/MoO2 composite with a flower-like structure for high-performance lithium-ion batteries (LIBs). MoSe2 could lead to fast and facile movement of Li+ due to its larger interlayer spacing. Meanwhile, MoO2 could protect the lamellar structure of MoSe2 from being destroyed in the charging/discharging processes to maintain the required active surface to electrolytes. In addition, the flower-like structure of the composite could effectively alleviate the volume expansion during charging/discharging. As LIBs are anode material, MoSe2/MoO2 composite demonstrates an excellent specific discharge capacity of 1042 mAh g−1 after 100 cycles at 0.1 A g−1, which is attributed to the synergistic effects of MoSe2 and MoO2 in the composite.