CaZnOS-based semiconductors are the only series of material system discovered that can simultaneously realize a large number of dopant elements to directly fulfill the highly efficient full-spectrum functionality from ultraviolet to near-infrared under the same force/pressure. Nevertheless, owing to the high agglomeration of the high temperature solid phase manufacturing process, which is unable to control the crystal morphology, the application progress is limited. Here, the authors report first that CaZnOS-based fine monodisperse semiconductor crystals with various doping ions are successfully synthesized by a molten salt shielded method in an air environment. This method does not require inert gas ventilation, and therefore can greatly reduce the synthesis cost and more importantly improve the fine control of the crystal morphology, along with the crystals’ dispersibility and stability. These doped semiconductors can not only realize different colors of mechanical-to-optical energy conversion, but also can achieve multicolor luminescence under low-dose X-ray irradiation, moreover their intensities are comparable to the commercial NaI:Tl. They can pave the way to the new fields of advanced optoelectronic applications, such as piezophotonic systems, mechanical energy conversion and harvesting devices, intelligent sensors, and artificial skin as well as X-ray applications.