Surplus tetracycline in the water body causes damage to the ecology balance and human health. Therefore, this work established an efficient strategy, namely, the BFO-based UV-heterogeneous Fenton-like system, to eliminate TC pollution. The photocatalytic oxidation system has been integrated with the heterogeneous Fenton-like system, cooperated with the photolysis of H2O2. These synergistic effects could boost the generation of reactive species for the TC degradation and mineralization, due to the reduction of Fe(III) to Fe(II) by photogenerated electrons and the separation of photogenerated electron-hole pairs. The prepared BFO was stable with no secondary pollution, and could be recovered by an extra magnet to reuse. Compared with other single oxidation systems, this coupled system showed an outstanding performance in TC disposal, and TC and TOC removal efficiencies could reach 100% and 74.92%, respectively. Moreover, the mechanisms for TC degradation involved that TC was degraded by oxidation species, such as superoxide radicals, hydroxyl radicals, and positive holes, and intermediate products in the TC degradation process mainly were products at m/z = 459, m/z = 445, and m/z = 134. The promising TC disposal efficiency achieved by the integration between BFO-based photocatalytic and heterogeneous Fenton-like system sheds light on applying BFO to control water pollution.