One of the key principles of rational environmental management is finding ways to recycle by-products. Gypsum-bearing waste such as phosphogypsum (PG) is a large-scale waste. Resolving the problem of its accumulation is a global challenge. Phosphogypsum is a by-product of orthophosphoric acid and phosphate fertilizer production. PG mainly consists of calcium sulfate dihydrate and can be considered as an alternative to natural gypsum rock in gypsum binder production. However, previous studies have shown that the structural and morphological features of PG particles are the cause of the high water demand of phosphogypsum binders (PGB) and the resulting low physical and mechanical properties of consolidated phosphogypsum paste. This study examined the possibility of increasing PGB efficiency by increasing their dispersion, including by grinding. The study found that grinding PGB after calcination generally improves its properties and can be recommended as an effective manufacturing technique for reducing the impact of the structural and morphological properties of phosphogypsum from various sources on the quality of the final product. The compressive strength of PGB after grinding to a specific surface area of ≈480 m2/kg ranged from 3.06 to 5.41 MPa after 2 hours of mixing and from 6.78 to 13.68 MPa in the dry state.