It is necessary to effectively separate photocatalytic materials from water bodies and reuse catalysts for industrial wastewater treatment. Herein, a novel nanofiber membrane with enhanced light absorption and reusability of photocatalytic materials was prepared. The three-dimensional porous structure of the nanofibers helps the photocatalyst efficiently degrade pollutants. Specifically, a high-efficiency photocatalyst carrier with a nanofiber structure (PAN/PU/β-CD@Ag nanofiber membrane) was prepared by electrospinning and a simple silver plating process, and then ZnO NPs were synthesized in situ on the nanofiber membrane during the hydrothermal process. Under visible-light irradiation, the ZnO-loaded PAN/PU/β-CD@Ag nanofiber membranes exhibited excellent photocatalytic performance for the degradation of methyleneblue (MB, 71.5%) and tetracyclinehydrochloride (TCH, 70.5%). Additionally, a possible pathway of charge migration in this system was proposed. This design may provide a new idea for the preparation of visible-light photocatalytic nanofiber membranes and their treatments of wastewater containing dyes and hormones.