The cotton cellulose nanofibers(CCNFs)/ZnO/CuS nanocomposites have been successfully fabricated by the electrospun-hydrothermal method and successive ionic layer adsorption. The results of XRD, SEM and TEM indicate that the CuS are successfully combined with the ZnO. The photocatalytic activity of the CCNFs/ZnO/CuS nanocomposites is investigated by the degradation of methylene blue under visible light irradiation, and it is demonstrated to be significantly enhanced after the CuS is introduced. Furthermore, the direct interfacial charge transfer of the ZnO/CuS is considered as the main reason for the enhancement.