A novel magnetic MIL-101(Fe)/TiO2 composite was synthesized for photo degradation of tetracycline (TC) under solar light. The composite was characterized by XRD, TGA, SEM, TEM, EDS, BET, FTIR, XPS, VSM, ESR, and PL. The resultant composite was environment friendly material, which exhibited high TC degradation efficiency and excellent reusability. In the meantime, it could be separated easily from TC solution by using magnet, which would save significant time and cost of preparation and degradation, having broad prospect in application. Using 1 g L-1 magnetic MIL-101(Fe)/TiO2 at pH = 7, 92.76% degradation efficiency was achieved under solar light irradiation in 10 min for 20 mg L-1 TC. Further experiments indicated that TiO2 introduced in the composite played an important role in the degradation process, which could be activated by the UV light in solar light to generate large amount of center dot O-2(-) and center dot OH radicals. The degradation efficiency of TC in this paper was significantly higher than other research papers reported in last three years. This study put forward new magnetic Fe-based metal-organic frameworks (MOFs)/TiO2 composite for degrading pharmaceutical wastewater.