The mixed Al-Fe pillared bentonite (Al/Fe-B) was tested as a heterogeneous catalyst for the photo-Fenton discoloration of azo dye X-3B under solar light irradiation. The structural characteristics of the catalyst were examined by XRD, BET, and TEM. The results indicate that the heterogeneous photo-Fenton process employing the Al/Fe-B as catalyst exhibits higher photo-catalytic activity compared to its corresponding homogeneous photo-Fenton process. The amount of Fe ions in solution leaching from the Al/Fe-B is less than 0.26% of the total iron content in the catalyst.