Calcium sulfate hemihydrate whiskers (CSHWs) were prepared from high-purity salt gypsum in a glycerol–water system. The effects of the glycerol/water ratio, reaction temperature, reaction time, and stirring speed on the crystal morphology of the CSHWs were investigated. Results showed that the average length and average length/diameter (L/D) ratio of the CSHWs first increased and then decreased as the glycerol/water ratio, reaction time, and stirring speed were increased, but they continued to gradually increase with increasing reaction temperature. The CSHWs had the highest L/D ratio and smooth surfaces—with an average length of 42.91 μm, an average diameter of 0.72 μm, and an average L/D ratio of 55—when the preparation conditions were a glycerol/water ratio of 2.0, a reaction temperature of 100 °C, a reaction time of 2.0 h, and a stirring speed of 300 rpm. This study provides a feasible idea for the treatment of salt gypsum, which achieves high value-added utilization of salt gypsum as well as the elimination of solid waste.