CdS materials have shown promise in optical refrigeration. However, the current success of laser cooling is still limited to nanobelt morphology. It is, therefore, important to explore whether bulk crystal growth technology could provide high-quality materials for laser cooling studies. Herein, we have demonstrated CdS bulk crystal growth by a modified optical floating zone method. The low temperature and continuous displacement of the CdS crystalline zone have resulted in high-quality CdS bulk crystals, which show strong photoluminescence upconversion with the absence of the long-wavelength and broad emission centered that commercial CdS wafers usually exhibit. All these characterizations have confirmed the excellent stoichiometric nature and crystal quality of CdS bulk crystals, which is much better than the commercial counterparts for laser cooling studies.