With the rapid development of nuclear-related industries in the world, the consequent environmental pollution of radionuclides has become an increasingly serious problem due to the great harm to environmental diversity and human health. The photocatalytic removal of radionuclide on CdS-based photocatalysts has been attracted widely attentions due to the suitable band gap and high photocatalytic efficiency. In this study, approximately 97.5% of U(VI) was photo-catalytically reduced into U(IV) by 2.5 wt% MoS2/CdS composite within 15 min. After 5 cycles, 2.5 wt% MoS2/CdS composite still exhibited the high removal efficiency of U(VI) under 50 min irradiation, indicating the good stability. The findings indicated that CdS-based catalyst has a great potential for the photocatalytic reduction of uranyl in actual environmental remediation.