Hydrogen-terminated diamond (H-diamond) metal oxide field effect transistors (MOSFETs) were successfully fabricated on polished first-grown and unpolished secondary-grown silicon-based polycrystalline diamond films. The devices have a gate length of 8 μm, while an Al2O3 dielectric bilayer was deposited at 200 °C and 100 °C using atomic layer deposition (ALD). Compared to the first-grown diamond films with a root-mean-square roughness (Rq) of 257 nm, the films after polishing and subsequent second growth change the diamond growth mode, resulting in a mixed surface morphology characterized by faceted and step-bunching structures with a roughness (Rq) of 16.6 nm, and also leading to a decrease in grain boundary density and polishing-induced defects. Device analysis demonstrates that these changes result in an increase in the on/off ratio from 102 to 107 at a gate leakage current of 10−7 mA/mm. Meanwhile, although polished first-grown diamond films have atomic-level smoothness, the devices channels on unpolished secondary-grown diamond films show higher carrier concentration and mobility. The improvement in device performance indicates that the three-step growth method provides a new opportunity for the application of large-sized silicon-based polycrystalline diamond films in electronic devices.