High-intensity crop-production seeking for higher grain yields increases nutrient demand by plants. A field experiment was performed in Parana State, Brazil, on a clayey Haplic Cambisol to evaluate the effects of phosphogypsum and nitrogen (N) amendments on a wheat–soybean rotation. Phosphogypsum was surface-applied to plots at 0, 2, 4, and 6 Mg ha−1 before wheat sowing and two rates of urea at 40 and 80 kg N ha−1 were applied to subplots in top dressing at tillering of wheat. Phosphogypsum improved the yield performance of wheat–soybean rotation. Wheat grain yield increased by 20% due to phosphogypsum application only when a higher rate of urea at 80 kg N ha−1 was applied in top dressing, indicating an influence of the interaction between N and sulfur (S). Soybean grain yield increased by 16% with phosphogypsum application, regardless of the urea-N rates to the previous wheat crop. Higher grain yields of wheat and soybean were related to higher levels of Ca2+ and S in the soil profile (0–0.40 m). Although there was a slight involvement of phosphogypsum in reducing aluminum Al3+ toxicity in the subsoil due to a reduction in Al3+ saturation caused by increased Ca2+ concentration, the improvements imparted by the use of phosphogypsum resulted mainly from increased S concentration. The results showed that the critical levels of SO4–S by 0.01 mol L−1 Ca(H2PO4)2 were 14 and 27 mg dm−3 at 0–0.20 m and 0–0.40 m depths, respectively, for the wheat–soybean cropping system. [ABSTRACT FROM AUTHOR]