Herein, we report a novel 1/GO/FeO photocatalyst, comprising Ce(BTB)(HO) (MOF-1, HBTB = 1,3,5-benzenetrisbenzoic acid), graphene oxide (GO), and iron oxide (FeO) for photocatalytic degradation of chlortetracycline (CTC). This design enables the effective transfer of electrons from the MOF to GO, thereby reducing the photoelectron-hole recombination rate. Therefore, the optimized 1/GO/FeO photocatalyst with HO shows the highest photocatalytic activity toward CTC. The kinetic constant is 5.4 times that in the system of MOF-1 and hydrogen peroxide, which usually acted as efficient electron acceptors to improve the photocatalytic performance of MOFs. More importantly, light absorption is extended from the ultraviolet to the visible region. Furthermore, 1/GO/FeO can be quickly recycled under an applied magnetic field and displays outstanding stability and reusability. According to the radical trapping experiments and electron paramagnetic resonance results, hydroxyl radicals, superoxide radicals, and holes all contribute to excellent photocatalytic activity. The possible catalytic mechanism of 1/GO/FeO is tentatively proposed. This work aims to explore the synergistic effect between metal-organic frameworks (MOFs) and GO, and provide a theoretical basis for MOF-based composites to remove antibiotic contaminants in the environment.