We report the enhanced charge storage characteristics of ultrananocrystalline diamond (UNCD) by contact electrification-induced hydrogenation. The non-catalytic hydrogenation of UNCD films was achieved by using platinum as an electron donor and sulfuric acid as a hydrogen proton donor, confirmed by Raman spectroscopy and time-of-flight secondary ion mass spectroscopy (TOF-SIMS). Chemical treatment with only a H2SO4 solution is responsible for the surface oxidation. The oxidation of UNCD resulted in an increase in the quantity and duration of the tribocharges. After non-catalytic hydrogenation, the generation of friction-induced tribocharges was enhanced and remained for three hours and more. We show that the hydrogen incorporation on grain boundaries is responsible for the improvement of charge storage capability, because the doped hydrogen acts as a trap site for the tribocharges. This lab-scale and succinct method can be utilized to control charge trap capability in nanoscale memory electronics.