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A single crystal of potassium tantalum niobate was chosen to deposit high quality diamond thin films by microwave plasma chemical vapor deposition (MPCVD) techniques. The surface morphologies and microstructures of the as-deposited diamond films were characterized by XRD, SEM, and Raman spectroscopy. The photocatalytic properties of the samples were studied. A TaC transition layer was identified during the deposition of diamond. Additionally, it was observed that as the deposition time prolonged, the quality of the diamond film improved. All film samples showed good ability to degrade Rhodamine B, with the degradation rate of the film deposited for 12 h being 0.29 times higher, corresponding to a 1.6 times greater degrading speed of Rhodamine B compared to the film deposited for 3 h. This research introduces a novel substrate for depositing polycrystalline diamond and explores its application in photocatalysis.