In this work, an amino-functionalized Zr-based metal-organic polyhedron (denoted ZrT-1-NH2), synthesised under the solvothermal method, has been selected as the photocatalyst for the removal of tetracycline (TC). The effects of adding dosages, pH values of TC degradation efficiency were investigated, and the results showed that this material was better effective in photocatalysis degradation of tetracycline antibiotic. In addition, the trapping experiments reveal that hydroxyl radical (•OH) and superoxide radical (•O2−), serving as active species, play major roles in the photocatalytic process. Furthermore, a possible mechanism for the photocatalytic process is proposed. This work presents that zirconium-based metal-organic polyhedra (Zr-MOPs) may be promising photocatalysts for the removal of antibiotics in wastewater.