The catalytic wet peroxide oxidation (CWPO) of toluene on two bentonite-based AlFe-pillared clays (PILCs) with different iron contents was investigated. The PILCs were obtained using bentonite clay from Bogovina, Serbia. The change in chemical and phase composition and textural properties of the starting clay and synthesized catalysts was monitored using X-ray diffraction, inductively coupled plasma optical emission spectrometry, UV-Vis diffuse reflectance spectrometry, and physisorption of nitrogen. The catalytic performance was examined using gas chromatography. The Na-exchange process lowered the (001) smectite basal plane spacing, but the clay retained its swelling properties, while the pillaring process increased it. The surface areas of both synthesized pillared clays increased to similar values although their Fe content was different. At 37 ℃, both catalysts show significant toluene degradation, with the one richer in Fe having higher efficiency. The leaching of the active cations during reaction was negligible, and the catalysts were stable. AlFe-pillared clay catalysts can be used in CWPO for the elimination of BTEX compounds from plant effluent streams.