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.