A field experiment was conducted at farmer's field in Mollisols of Tarai soils in Uttarakhand (India), to assess the direct and residual effect of sulfur fertilization in wheat-soybean cropping sequence. Four levels of sulfur (S; 0, 15, 30, and 45 kg ha⁻¹) were applied to main crop (wheat) along with recommended dose of nitrogen (N), phosphorous (P), and potassium (K). The direct and residual effect of sulfur at highest level showed 27 and 6 percent increase in grain yield of wheat and soybean over control, respectively. The increase in grain yield of wheat was significant at each sulfur level. The direct as well as residual effect of sulfur showed significant increase in sulfur concentration and its uptake by grain and straw except increase in sulfur concentration and uptake by soybean straw. In wheat-soybean cropping sequence, the agronomic efficiency and apparent sulfur recovery decreased with increase in levels of sulfur, but the percent response increased with increasing sulfur application. Different forms of sulfur such as total sulfur, organic sulfur, calcium chloride extractable sulfur, potassium dihydrogen phosphate extractable sulfur, and non-sulfate sulfur in post-harvest soil increased according to sulfur level applied but it decreased under control and also after residual crops. The buildup of sulfur in surface soils was greater than in the deeper soils. Application of sulfur showed the positive sulfur balance and it increased with increase in sulfur level, while it was negative under control. A major portion (46–62%) of applied sulfur contributed to increase in sulfur content of root zone soil followed by unaccounted component (25–40%) and small portion (11–18%) was absorbed by wheat plant as uptake.