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Eco-friendly pillared montmorillonites, in which the pillars consist of iron oxide, are expected to have interesting and unusual magnetic properties that are applicable for environmental decontamination. A completely "green" and effective composite was synthesized using mild reaction conditions and benign products. The composite was characterized by scanning electron microscopy (SEM) equipped with EDS, transmission electron microscopy (TEM), X-ray diffraction (XRD), and thermogravimetric analysis (TGA). Catalytic activity was tested against the degradation of dichlorophenol (DCP) and was found that in the presence of peroxymonosulfate 85% of DCP disappeared in 2.5 h, whereas in the presence on hydrogen peroxide and peracetic acid nearly 50% and 70% of DCP, respectively, degraded in 3.5 h. TOC showed about 85% demineralization of the solution, which indicates a successful degradation of DCP.