light-generators, stress sensing, flexible, and stretchable displays, mechanical energy harvesting and conversion, and integrated tribotronic devices. [1][2][3][4][5][6][7][8][9][10] They can emit light and are regarded as smart creatures (like Noctiluca scintillans shining by the impact of waves) when exposed to external momentary stimuli. [11][12][13][14] Many materials discovered in nature provide the capability to emit light in response to dynamic forces/pressures, whether natural or man-made, such as quartz and sugar. [15,16] There are two categories of ML materials systems: organics and inorganics; [17,18] however, most of the current organic ML materials emit photons by releasing energy from the breaking of chemical bonds, resulting in a poor recovery, or requiring recrystallization to reproduce the light emitting process. Inorganic ML materials can be divided into insulators and semiconductors. As one of the II-VI ML semiconductors, ZnS has very interesting mechanical-to-optical properties, owing to its labile changing elastic and plastic deformation crystal structure, as well as its special piezoelectric and friction characteristics. [19][20][21][22][23][24] The novel ML properties of ZnS-based composites have aroused broad research interest in recent years. [1,[26][27][28][29][30][31] Semiconductors such as doped ZnS, can directly convert mechanical energy into light energy, providing broad application prospects in the fields of stress/strain sensing, wind/droplet driving displays, 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.