The article is devoted to the study of the influence of residual sulfuric and phosphoric acids on the process of processing large-tonnage phosphogypsum (PG) waste into calcium carbonate. In the Russian Federation, about 10 percent of existing phosphogypsum waste is processed into construction materials. Acidic impurities (phosphoric and sulfuric acids) in their composition are an obstacle to the use of phosphogypsum for the production of binders. This study finds that impurities also reduce the chemical activity of phosphogypsum. At the same time, the paper focuses on the potential of phosphogypsum for the production of calcium carbonate. This article investigated the amount of impurities in phosphogypsum. The results show that during automatic washing of phosphogypsum, losses are approximately 30–35 wt. %. It was also found that phosphogypsum by 22% consists of impurities of phosphoric and sulfuric acid. These acids are characteristic waste products of extraction phosphoric acid (EPA) production. By ASTM C471M-20ae1, the content of calcium sulfate dehydrate and hemihydrate before and after washing was determined. A thermodynamic calculation of the proposed interaction of phosphogypsum with carbonates showed that the characteristic reaction is possible. The conversion process of phosphogypsum to get the corresponding calcium carbonate was carried out at 70 °C. Data on the chemical composition of the reaction products, obtained by X-ray fluorescence analysis on a Shimadzu EDX-7000 spectrometer, showed that some reactions proceed incompletely and need the selection of optimal conditions. The potential commercial benefits of processing phosphogypsum by carbonization were defined for products such as calcium carbonate or its derivatives.