In order to further develop efficient ultraviolet light-driven photocatalysts for environmental application, α-zirconium phosphate (α-ZrP) and carbon nitride (C3N4) were synthesized, respectively. Then, C3N4-ZrP compositing nanomaterials were prepared by compositing α-ZrP nanocrystals and C3N4 with different mass ratios. C3N4-ZrP compositing nanomaterials were characterized by X-ray diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. The results illustrated that α-ZrP and C3N4 were successfully composited, and the polarization of the compositing nanomaterials was reduced compared with raw materials. The photocatalytic performances of C3N4-ZrP compositing nanomaterials with different mass ratios were studied by photodegradation of RhB under ultraviolet irradiation. All of the degradation rates of the C3N4-ZrP compositing nanomaterials system were achieved more than 90% after 18 min. When the mass ratio of C3N4-ZrP compositing nanomaterials is 2:1, the degradation efficiency achieved 99.95%, which is more efficient than other tested mass ratios. The result indicated the possibility of utilizing C3N4-ZrP compositing nanomaterials for environmental pollutants degradation.