Particle shape plays an important role in flotation. The strategy of regulating particle morphology during crystallization process to make it more suitable for flotation was proposed. Crystalline particles were more regular than ground particles, and mainly in a cubic-like shape. The results of micro flotation tests indicated that crystalline samples floated better than ground samples in a wide size range. Adsorption capacity tests suggested that there was almost no difference in the adsorption amount of SDBS between ground and crystalline sample. Morphology analysis and bubble-particle attachment experiment demonstrated that the geometric features of crystalline particles facilitated the longer three-phase lines, making the attachment between crystalline sample and bubble more stable, which could be thought as the main reason for the higher floatability of crystalline sample. The novel strategy called "crystal-regulation flotation" could provide an innovative idea for the flotation of soluble potassium salt and promote the development of flotation technology.