We report improved the triboelectric properties of ultraviolet (UV)-irradiated ultrananocrystalline diamond (UNCD) films that were measured using atomic force microscopy (AFM). Fabricated using the chemical vapor deposition (CVD) method, UNCD is an artificial diamond film with mechanical properties similar to single-crystal diamond. Surface modification by means of UV irradiation is a simple method to modify the surface properties of carbon-based and oxide materials. While the physical properties (e.g., roughness, adhesion, and friction) of these UNCD films did not exhibit any significant change following the UV treatment, we found that the UV-irradiated UNCD surface was oxidized and became graphitic, as confirmed using X-ray photoelectron spectroscopy, work function measurements using Kelvin probe force microscopy, and ultraviolet photoelectron spectroscopy. The work function of the samples increased with increasing UV exposure time, which is associated with the reduction of carbon atoms on the surface and oxygen-rich surfaces. Tribocharges were generated by scratching the surface of the UNCD films with a diamond-coated AFM tip. The duration of the tribocharges increased because of reactive radicals and the insulating property resulting from the UV/ozone treatment. The radicals were responsible for trapping charges; the UV-irradiated UNCD films preserved the charges for more than 5 h, which is five times longer than that on bare UNCD. This study demonstrated that UNCD is a promising material for generating triboelectricity and that UNCD can be used as a charge-trapping layer in charge-trap flash memory devices.