Every year, the production of industrial phosphoric acid generates more than 100 Tg of phosphogypsum (PG), leading to significant environmental damage and the occupation of a vast amount of land space. The urgent need to explore applications for PG has become increasingly apparent. However, impurities such as organic substances, slime, phosphorite, and SiO2 reduce the whiteness of PG, making it difficult to utilize for high-value applications. To address this issue, this study employed a two-stage flotation process to remove the majority of impurities, including SiO2, organic substances, and fine slime adhered to the surface of PG particles. The raw PG sample was first sieved to remove some SiO2 particles. After flotation, sulfuric acid and tributyl phosphate were introduced to decompose the PG particles and remove the impurities wrapped inside. Following this flotation combined extraction process, the whiteness of the PG sample improved from 54.1% to 92.9%, meeting the requirements for building walls and filters.