The Mn-doped ZrO 2 /TiO 2 nanostructured photocatalysts had been prepared by the simple hydrothermal method. The morphologies and structures of the as-prepared photo-catalyst were characterized by transmission electron microscopy, x-ray diffraction, x-ray photoelectron spectroscopy, and electron paramagnetic resonance. The resultant nanostructured photocatalysts exhibited high photocatalytic activity under ultraviolet (UV) light irradiation, attributing to the improvement of the photo-absorption property and the separation efficiency of photogenerated electrons and holes. The hydroxyl radicals (•OH), superoxide radical (•O 2 − ), and holes (h + ) are the main active species in aqueous solution under UV light irradiation.