High-quality polycrystalline diamond films with dominated (100)-oriented grains are realized by combining the thermally oxidation and the homogeneous second growth processes. Moreover, we investigate the wettability property of the polycrystalline diamonds in various stages. Different surface structures (with various grain sizes, voids, and orientations, etc.) and terminations (hydrogen or oxygen) have significant effects on the wettability of polycrystalline diamond films. The wettability is further closely related to the polarity of solutions. By measuring the contact angle and calculating the dispersion and polarity components, we estimate the surface energy of polycrystalline diamond films, and explore the factors affecting the surface energy. The modulations in growth quality and wettability property of polycrystalline diamond films provide valuable data for development of diamond-based multiple devices in practical applications.