Recently, cadmium selenide (CdSe) has been deeply studied because of its excellent photocatalytic hydrogen (H-2) production performance. However, pure CdSe has poor stability and severe photocorrosion, which seriously affect its application prospect. In this work, we successfully deposit Bi2MoO6 on an inorganic-organic CdSe-diethylenetriamine (DETA) hybrid to design Bi2MoO6/CdSe-DETA composites by an in situ solvothermal method. The morphology, crystal structure, electrochemical properties, H-2 evolution performance and the photostability of Bi2MoO6/CdSe-DETA composites are explored using various techniques. The results show that the as-prepared Bi2MoO6/CdSe-DETA composites exhibit excellent photocatalytic performance and photostability under visible light irradiation. Among them, the Bi2MoO6/CdSe-DETA hybrid system exhibits excellent photocatalytic H-2 production performance (5.92 mmol g(-1) h(-1)), which is approximately 3.6 and 1.8 times higher than that of pure CdSe and CdSe-DETA, respectively. After 4 cycles, the photocatalyst still maintains high H-2 production. This study develops a new type of photocatalyst that can respond to visible light. This provides an effective way to solve the energy problem by using solar energy.