A good design of efficient metal-organic framework material (MOF)-based photocatalysts with high intrinsic activity for tetracycline (TC) is highly desirable, but challenging, for water purification. Herein, we have constructed a novel TiO2@UiO-66-NH2 nanocomposite through a convenient one-step solvothermal technique. The TiO2@UiO-66-NH2 nanocomposite displayed outstanding adsorption and photodegradation performances toward TC in aqueous solution under restricted space and visible light illumination. The improved catalytic ability was mainly caused by the enhanced adsorption property and the successful transfer of photogenerated electrons to the conduction band of TiO2@UiO-66-NH2. Importantly, the photocatalyst efficiency was not tremendously decreased even after the fourth round of recycling, indicating its good stability and reusability. We believe that our study could be conducive to the future design and accomplishment of MOF surface interactions with organic pollutants, expanding the application of MOFs and photocatalysts for elimination of pollutants from wastewater.