Field experiments were carried out at Oilseed Research Farm, Kalyanpur, Kanpur with mustard variety Varuna and at Fertilizer Research Station, Uttaripura, Kanpur on sesame variety T-78 both under C. S. Azad University of Agriculture & Technology, Kanpur, Uttar Pradesh (India) during 2013–14 to evaluate the response of polysulphateon yield and quality of mustard and sesame. Results of the experiments revealed that use of polysulphate as a source of sulphur significantly increased grain and stover yield of both the crops up to 100% sulphur level. Oil content in both the crops also significantly enhanced due to use of polysulphate up to 100% level of sulphur through polysulphate. Maximum grain yield of mustard and sesame crops was 25.20 and 11.10 q/ha with oil content of 43.45 and 45.50%, respectively, under T5 [100% NP+100% S through polyphosphate (Balanced K through MOP to make 100% K)]. Polysulphate proved its superiority over gypsum at 100% level of sulphur used.