In this study, the photocatalytic activity of pure Fe-doped ZnO and Fe-doped ZnO/Montmorillonite nanocomposite has been investigated for the degradation of malachite green under UV light irradiation. Both photocatalysts were synthesized using co-precipitation method and characterized by X-ray diffraction, energy dispersive X-ray spectroscopy, Fourier-transform infrared absorption, and electron spin resonance. The results showed that the photocatalytic efficiency is better in the presence of montmorillonite compared to pure Fe-doped ZnO. To detect the possible reactive species involved in degradation of organic dyes control experiments with introducing scavengers into the solution of organic dyes were carried out. It is found that electron plays an important role in the degradation of malachite green.