Fe-Co bimetallic oxides supported on mesoporous zirconia (Fe-Co/ZrO2) was prepared using incipient wetness co-impregnation method and characterized by transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy and UV-vis diffuse reflectance spectra. Compared with individual component Fe or Co catalysts, Fe-Co/ZrO2 exhibited higher ozonation efficiency for the degradation of the tested toxic pollutants, as demonstrated with the herbicides 2,4-dichlorophenoxyacetic acid and pharmaceutical phenazone, diphenhydramine hydrochloride in aqueous solution. Furthermore, the characterization studies indicated that Fe-Co oxides were highly dispersed on the surface of mesoporous zirconia with multivalent oxidation states. The interfacial electron transfer process was greatly enhanced due to the presence of two redox couples (Fe3+/Fe2+ and Co2+/Co3+) in Fe-Co/ZrO2, which caused the higher catalytic reactivity for ozone decomposition into (OH)-O-aEuro cent radicals, leading to the efficient removal of toxic pollutants in aqueous solution. The catalytic mechanism of pollutants degradation over Fe-Co/ZrO2 with ozone was proposed on the basis of all information obtained under different experimental conditions. The multivalent oxidation states, high dispersion and the synergistic effect of Fe-Co oxides in Fe-Co/ZrO2 enhanced the interfacial electron transfer process, which caused the higher catalytic reactivity for the degradation of toxic pollutants in aqueous solution.