In this paper, two dielectric layers of Al2O3 and Gd2O3 were prepared by an atomic layer deposition (ALD) and magnetron sputtering deposition (SD), respectively. Based on this, a metal-oxide-semiconductor field-effect transistor (MOSFET) was successfully prepared on a hydrogen-terminated single-crystal diamond (H-diamond), and its related properties were studied. The results showed that this device had typical p-type channel MOSFET output and transfer characteristics. In addition, the maximum current was 15.3 mA/mm, and the dielectric constant of Gd2O3 was 24.8. The effective mobility of MOSFET with Gd2O3/Al2O3 was evaluated to be 182.1 cm2/Vs. To the best of our knowledge, the bilayer dielectric of Gd2O3/Al2O3 was first used in a hydrogen-terminated diamond MOSFET and had the potential for application.