In this work the mixed Al-Fe pillared bentonite was developed and tested as a heterogeneous catalyst for the photo-Fenton oxidation of phenol under solar light irradiation. The structural characteristics of the catalyst were examined by X-ray diffraction (XRD) and scanning electron microscopy (SEM). The Al-Fe pillared clay exhibits higher basal distance than original bentonite. The effect of pH to the degradation of phenol and the reusability of the catalyst were addressed.The results of photocatalytic experiments indicate that the heterogeneous photo-Fenton process employing the Al-Fe pillared clay as a photocatalyst possesses a high potential for phenol degradation. During the photocatalytic reaction, the amount of iron leaching out increases as a function of time. Significantly lower concentration of Fe 2+ and Fe 3+ in the solution after the treatment could give a great advantage to the mixed Al-Fe pillared bentonite/H2O2 system over the homogeneous Fenton system.