Elegant integration of three-dimensional (3D) boron nitride (BN) into the porous structure of a polymer nanofiber (NF) membrane system results in a surface with enhanced absorption capacity for removal. Various BN-based applications were designed and developed successfully, but BN-based absorption systems remain relatively unexplored. To develop a reusable absorption strategy with high removal efficiency, we used a composite of 3D BN and polyacrylonitrile (PAN) to prepare a NF membrane with a porous structure by using electrospinning and spray techniques (BN-PAN ES NFs). The removal efficiency of the 3D BN NF membrane was higher than that of a pure carbon NF membrane. Water pollutants, such as the dyes Congo red (CR), basic yellow 1 (BY), and rhodamine B (Rh B), were tested, and the absorption ratios were 46%, 53%, and 45%, respectively. Furthermore, the aforementioned dyes and pollutants can be completely eliminated and removed from water by heating because of the high heat resistance of 3D BN. The membrane can be recycled and reused at least 10 times. These results indicate that BN-PAN ES NFs have can be used in water purification and treatment for absorption applications, and that they can be reused after heat treatment.