ZnO/ZnS core/shell nanocrystals (~5-7 nm in diameter) with a size close to the quantum confinement regime were successfully synthesized using polyol and thermolysis. X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) analyses reveal that they exist in a highly crystalline wurtzite structure. The ZnO/ZnS nanocrystals show significantly enhanced UV-light emission (~384 nm) due to effective surface passivation of the ZnO core, whereas the emission of green light (~550 nm) was almost negligible. They also showed slight photoluminescence (PL) red-shift, which is possibly due to further growth of the ZnO core and/or the extension of the electron wave function to the shell. The ZnO/ZnS core/shell nanocrystals demonstrate strong potential for use as low-cost UV-light emitting devices.