In this paper, the solid waste desulfurization gypsum produced by coal-fired power plants was used as a raw ma-terial to prepare calcium sulfate whiskers with high application prospects. Calcium sulfate whiskers with uniform morphology and high aspect ratio can be prepared by hydrothermal method in sulfuric acid solution. A new pro-cess of desulfurization gypsum activated by high-energy grinding to reduce the reaction temperature and sulfuric acid concentration was developed. Through the comparison of product morphology, the best grinding time was determined to be 3.5 h. The mechanism of desulfurization gypsum through physical–chemical coupling to reduce energy consumption was clarified. The activation of desulfurization gypsum by grinding and the acidic environ-ment provided by the sulfuric acid solution made the calcium sulfate solution reached rapid saturation and accel-erated the nucleation rate. By calculating the conversion and crystallization rate of calcium sulfate whiskers, it was found that there were obvious"autocatalytic"kinetic characteristics during the crystallization process.