In this report, heterogeneous Fenton-like degradation activities of ofloxacin (OFL) were investigated with synergistic degradation effects of bimetallic Fe-Cu on ordered mesoporous silicon (Fe-Cu@MPSi). With the characterization such as XRD, TEM, SEM and N-2 sorption-desorption isotherms, Fe-Cu@MPSi showed ordered mesoporous structure, high BET surface area, uniform mesopore size (similar to 2.4 nm) and moderate pore volume (0.19 cm(3)/g). The Fe2O3 and CuO nanoparticles highly dispersed in the mesopore channels, and the surface of the catalyst. Owing to the enhanced mass and electron transfer properties of mesoporous silicon, the synergetic interfacial effect of Fe and Cu on the surface of the catalyst and the complexation of OFL and Cu2+, the Fe-Cu@ MPSi heterogeneous Fenton-like catalyst showed exclusive and high degradation activities for OFL. The degradation mechanism of Fe-Cu@MPSi was also investigated with the optimal oxidation conditions of 30 mg/L OFL, 1 g/L catalyst, 2000 mg/L H2O2 and initial pH.