The low cost, natural origin, high stability, and great versatility for applications in adsorption and catalysis have made pillared interlayered clays (PILCs) one of the families of functional materials most intensively studied in the past three decades. PILCs involving several transition metals like Fe, Cu, or Mn are emerging nanomaterials exhibiting exceptional physicochemical properties. Besides, they also display excellent performance in the heterogeneous catalytic depletion of organic pollutants in aqueous systems. The recent literature involving these materials is reviewed, emphasizing on the works describing their role as active solids in the catalytic wet (hydrogen) peroxide oxidation (CWPO - CWHPO) of harmful organic compounds in contaminated aqueous streams.