Muscovite loaded Cu2O nanosphere composites with Fe3+ doping and Ag deposition were successfully synthetized by a simple chemical reduction method. The composites were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR) spectrometer, scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET) technique, transmission electron microscope (TEM), photoluminescence spectra (PL) and UV–Vis diffuse reflectance spectroscopy (UV–Vis DRS). Meanwhile, the photocatalytic performance and photocatalytic mechanism of the samples were investigated by photodegradation of methyl orange (MO) dye under visible light irradiation. The Cu2O nanosphere composites co-modified by Ag, Fe3+ and muscovite showed the best photocatalytic activity, which may originate from both the enhancement of utilization of Cu2O photocatalyst and the reduction of recombination of electrons and holes in the natural environment.