Introducing oxygen vacancies is an effective strategy to tail the absorption band-edge of ZrO2 photocatalyst into visible-light region and modifying its surface feature can promote the adsorption affinity toward organic molecules, resulting in the enhancement of visible-light photocatalytic degradation of organic pollutants. Herein, we prepared mesoporous ZrO2 with rich oxygen vacancy through a template-free solvothermal method followed by an annealing process, which was used as a catalyst to photodegrade tetracycline hydrochloride (TCH). The photocatalytic performance was found to be dependent on both oxygen vacancies and adsorption affinity. Comprehensive analysis revealed that, despite a certain reduction in both specific surface area and the amount of charged oxygen vacancy after annealing at 350 degrees C in air, the increased adsorption affinity toward TCH could promote its visible-light photocatalytic properties, along with good recyclability. Finally, a possible pathway and mechanism for the degradation of TCH was proposed.