Zinc oxide (ZnO) nanocrystals (NCs) were synthesized using a modified sol-gel method. Ultraviolet (UV) treatment was performed under various atmospheres on the highly stacked ZnO NCs. The prepared NCs were characterized using Fourier transform infrared spectroscopy, scanning electron microscopy, X-ray diffraction, photoluminescence spectroscopy, and atomic force microscopy to investigate their structural, electrical, and electrochemical properties. Through these analyses, the effect of the UV treatment on the chemical and electrical characteristics of ZnO NCs was established. According to the analyses, the organic ligands in the NCs were decomposed, and the particles were densified. The mobility of UV-treated ZnO NCs thin films increased to 1.4 cm2/Vs, almost 2 orders higher than the UV untreated ZnO thin films. It was confirmed that the recombination from oxygen vacancies of ZnO could be controlled by UV irradiation. As decreased oxygen vacancies, the band gap of ZnO NCs was increased from 3.2 eV to 3.27 eV.