A series of promising visible light driven ZnFe 2 O 4 modified Al 2 O 3 À MCM-41 nanocomposites were designed by wet impregnation method by loading different wt % (2, 6, 10) of ZnFe 2 O 4 on the surface of mesoporous Al 2 O 3 À MCM-41. All the prepared photocatalysts were analyzed by using X-ray diffractometers (XRD), Scanning electron microscope (SEM), N 2 sorption, Ultra violet-Visible Diffuse reflectance spectroscopy (UV-Vis DRS), Xray photoelectron spectroscopy (XPS), Fourier-transmission infrared spectroscopy (FTIR) and High-resolution transmission electron microscope (HRTEM) techniques to uncover and confirm the formation of phase, morphology and porous structure of the prepared nanocomposites. In the photo-Fenton reaction, the ZnFe 2 O 4 modified Al 2 O 3 À MCM-41 nanocomposites exhibit a significant catalytic activity for the photo-Fenton degradation of phenol (40 min, 99%) via photocatalysis and photocatalytic reduction of Cr (VI) (60 min, 66%) under sunlight with an excellent reusability nature. The high photo-Fenton activity of the composites is mainly attributed to mesoporosity and high surface area of support Al 2 O 3 À MCM-41, proper light harvestation and increased charge transfer efficiency by active species ZnFe 2 O 4 , and suitable band edge potential for hydroxyl radical generation. The photo-Fenton activities were further supported by the high photocurrent (0.29 mA/cm 2 ) generated by the nanocomposite ZnFe 2 O 4 modified Al 2 O 3 À MCM-41. These results open up a new route for ZnFe 2 O 4 modified Al 2 O 3 À MCM-41as an efficient photo-Fenton catalyst for environmental remediation with superior activity and higher stability.