A series of Fe-Al pillared bentonites with different Fe contents were synthesized through a simple ion exchange method. The samples were used as catalysts for the heterogeneous Fenton degradation of Orange II. The microstructure of the catalysts was characterized by X-ray diffraction (XRD), specific surface area measurements (SBET), Fourier transform infrared (FTIR) spectroscopy, Raman spectroscopy, and scanning electron microscopy (SEM). The obtained results showed that the pillaring process increased the basal spacing (d(001)) from 1.24 nm for the Na-bentonite (Bent) to 1.77 nm for the Al- Bent and ~1.72 nm for the Fe-Al pillared bentonites. The SBET values of the samples were increased after pillaring. It was obvious from the XRD and Raman results that intercalation was not achieved and that hematite was formed in the 20Fe-Al-Bent sample. The influence of Fe content on the degradation of Orange II was investigated. The catalytic activity of pillared bentonites increased with Fe content and hardly increased when the molar ratio of Fe/(Al + Fe) in the pillaring solution exceeded 10% . The decolorization efficiency and chemical oxygen demand (CODCr) removal of Orange II reached 100% and