We investigated how sulfur (S) application prior to wheat cultivation under wheat-rice rotation influences the uptake of cadmium (Cd) in rice grown in low- and high-Cd soils. A pot experiment was conducted with four S levels (0, 30, 60, 120 mg S kg⁻¹) and two Cd rates (low and high, 0.35 and 10.35 mg Cd kg⁻¹) supplied to wheat. Part of the wheat straw was returned to the soil before planting rice, which was cultivated for 132 days. To explore the key mechanisms by which S application controlled Cd accumulation in brown rice, (1) soil pore water at the key growth stages was sampled, and dissolved Cd and S species concentrations were determined; (2) rice plant tissues (including iron plaque on the root surface) were sampled at maturity for Cd and S analysis. With increasing S level, Cd accumulation in brown rice peaked at 60 mg S kg⁻¹, irrespective of soil Cd levels. For high-Cd soils, concentrations of Cd in brown rice increased by 57%, 228%, and 100% at 30, 60, and 120 mg S kg⁻¹, respectively, compared with no S treatment. The increase in brown rice Cd by low S levels (0–60 mg kg⁻¹) could be attributed to (1) the S-induced increase in soil pore water sulfate increasing the Cd influx into rice roots and (2) the S-induced increase in leaf S promoting Cd translocation into brown rice. However, brown rice Cd decreased at 120 mg S kg⁻¹ due to (1) low Cd solubility at 120 mg S kg⁻¹ and (2) root and leaf S uptake, which inhibited Cd uptake. Sulfur application to wheat crop increased the risk of Cd accumulation in brown rice. Thus, applying S-containing fertilizers to Cd-contaminated paddy soils is not recommended.