Spatially and spectrally resolved cathodoluminescence (CL) is one of the most effective methods to explore the optical properties of a nanomaterials and reveals the spatial distribution as well as the correlation between the luminescence and the sample morphology and microstructure. Here, CL modulation of ZnS nanostructures by controlled morphologies, Fe/Mn doping, and measurement temperature is demonstrated. High quality ZnS nanobelts and nanorods are synthesized on an Au‐coated Si substrate and an Au‐coated GaAs substrate via a facile thermal evaporation route. A room‐temperature sharp ultraviolet (UV) lasing‐like peak in various ZnS is achieved. The main UV luminescence peaks appear at wavelengths between 330 and 338 nm. The low temperature (32 K) CL spectrum consists of a narrow and strong UV peak centered at 330 nm and two broad, low‐intensity peaks in the visible region (514 and 610 nm). Temperature‐dependent CL from such single‐crystalline ZnS nanobelts in the temperature range of 32 to 296 K reveals two UV peaks at 3.757 and 3.646 eV. The effects of Fe doping and Fe/Mn co‐doping on the CL property of ZnS nanobelts are further investigated. These results imply that ZnS nanostructures can be used for potential luminescent materials as well as short‐wavelength nanolaser light sources.