Magnetically modified Fe-Al pillared bentonite (Fe3O4/ Fe-Al-Bent) was prepared via chemical co-precipitation method and characterized by powder X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), Fourier transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM). A series of experiments were carried out to investigate the degradation of Orange II by the obtained heterogeneous catalysts in the presence of H2O2. The experimental result indicated that the synthetic materials had a high catalytic activity and good reusability.