In this work, thin SiO₂ insulating layers were generated on the top and bottom surfaces of single-crystalline silicon plates (n type) by thermal oxidation to obtain an insulator/semiconductor/insulator (ISI) multilayer structure. X-ray diffraction (XRD) pattern and scanning electron microscope (SEM) pictures implied that all of the synthesized SiO₂ layers were amorphous. By controlling the thermal oxidation times, we obtained SiO₂ layers with various thicknesses. The dielectric properties of silicon plates with different thicknesses of SiO₂ layers (different thermal oxidation times) were measured. The dielectric properties of all of the single-crystalline silicon plates improved greatly after thermal oxidation. The dielectric constant of the silicon plates with SiO₂ layers was approximately 10⁴, which was approximately three orders more than that of the intrinsic single-crystalline silicon plate (11.9). Furthermore, both high permittivity and low dielectric loss (0.02) were simultaneously achieved in the single-crystalline silicon plates after thermal oxidation (ISI structure).