Rapid industrialization and ever-growing human activities have caused more and more serious water pollution in the last few decades, posing great threats towards both human health and ecological environment. Organic dyes, as one of the major water pollutants, are usually toxic, chemically stable, and hard to degrade. Photocatalytic technology, with its unique advantages, has become a focus of scientific research and is widely used in the treatment of organic pollutants in wastewater. In this paper, electrospinning technology was used to prepare visible light catalyst TPPZn/Ag3PO4 nanofiber and the morphology was studied by SEM. The TPPZn/Ag3PO4 nanofiber was used as both adsorbent and photocatalyst for removal methylene blue (MB) and rhodamine B (RhB). After 165 min of xenon lamp irradiation, the total removal rate of MB reached 99.05%, and after 300 min of irradiation, the total removal rate of RhB reached 94.85%. In addition, the reusability research shows that the TPPZn/Ag3PO4 material has stable performance and can be reused.