In this work, MoSe2-WS2 nanocomposites consisting of WS2 nanoparticles covered with few MoSe2 nanosheets were successfully developed via an easy hydrothermal synthesis method. Their nanostructure and photocatalytic hydrogen evolution (PHE) performance are investigated by a series of characterization techniques. The PHE rate of MoSe2-WS2 is evaluated under the white light LED irradiation. Under LED illumination, the highest PHE of MoSe2-WS2 nanocomposite is 1600.2 µmol g−1 h−1. When compared with pristine WS2, the MoSe2-WS2 nanostructures demonstrated improved PHE rate, which is 10-fold higher than that of the pristine one. This work suggests that MoSe2-WS2 could be a promising photocatalyst candidate and might stimulate the further studies of other layered materials for energy conversion and storage.