Metal-organic frameworks (MOFs) are a new class of porous crystalline materials being used as photocatalysts for efficient pollutant removal and environmental remediation. In this study, the TMU-32 MOF was synthesized as an effective photocatalyst for the photodegradation of tetracycline (TC) with 96% efficiency in 60 min under visible light. The high photocatalytic activity of the TMU-32 MOF is mainly due to its large specific surface area, which is beneficial for promoting both the adsorption of TC and the separation of the photoinduced charges. Moreover, its desired crystallinity makes it a semiconductor with an appropriate band gap energy. Next, a composite of the TMU-32 MOF with FeO nanoparticles (as FeO@TMU-32) was prepared as a magnetically recyclable photocatalyst. The results showed that the photocatalytic activity of the FeO@TMU-32 nanocomposite is slightly lower (68% degradation of TC within 60 min) than that of TMU-32 toward TC degradation since FeO nanoparticles are not acting as a photocatalyst and are used only to make the host photocatalyst (here, TMU-32) magnetically separable. The effects of the photocatalyst concentration and recyclability on the photodegradation of TC were studied under similar conditions. We found that the FeO@TMU-32 composite is easily recycled without a significant loss of photocatalytic activity after being used several times, indicating the stability of the photocatalyst. Finally, a density functional theory study was also conducted to investigate the structural and electronic properties such as the band gap energy and density of states of the TMU-32 MOF and the FeO@TMU-32 composite. Our computational results are in good agreement with the experimental ones. A photocatalytic degradation mechanism was finally proposed under visible-light photoirradiation.