In this work, from Bent-CD, refined bentonite (Bent-TC) was prepared using the wet method and the pillared bentonites Bent-Al, Bent-Al/Fe and Bent-Al/Cu were synthesized by the intercalation of AI, Al/Fe and Al/Cu polycation pillars into the interlayer channels of bentonite solid, respectively. The catalytic activity of these pillared bentonites was studied in oxidation reaction of phenol with hydrogen peroxide (H2O2) in aqueous solution at 40°C and atmospheric pressure. The obtained experimental results revealed that Bent-Al/Cu was the best catalyst. It can be interpreted that Bent-Al/Cu possesses large basal spacing (d001 and Cu likely is a good catalyst promoter for Al in order to generate more OH radials in that oxidation reaction.