The rice (Oryza sativa L.)- groundnut (Arachis hypogaea L.) is one of the most important cropping systems of Eastern India for human and animal diets. Both rice and groundnut benefit from sulphur application, but a major challenge in maintaining their growth, productivity and profitability is the widespread sulphur deficiency, affecting about 44% of Indian soils and 36% of soils in Odisha. A field experiment comprising five sulphur fertilisation strategies for rice viz., no sulphur, S @ 20 kg ha-1 through bentonite, S @ 20 kg ha-1 through gypsum, S @ 40 kg ha-1 through bentonite and S @ 40 kg ha-1 through gypsum allocated to main plots and three sulphur levels for groundnut viz., no sulphur, S@ 30 kg ha-1 and S @ 60 kg ha-1 allocated to the subplots was conducted in a split-plot design with four replications during the kharif and rabi seasons of 2021-22 and 2022-23 at Bhubaneswar, India to assess the effect of treatments on growth, productivity, quality and profitability of the component crops and the system. The application of S @ 40 kg ha-1 through gypsum to rice recorded the maximum values of growth parameters, biological yield, quality parameters and economics indices of rice, whereas the application of S @ 60 kg ha-1 in groundnut recorded the maximum values of growth parameters, biological yield and quality parameters of groundnut. Application of S @ 40 kg ha-1 through bentonite to rice combined with S @ 60 kg ha-1 in groundnut was the most remunerative with the maximum system net return (Rs. 113640 ha-1) and return per rupee investment (1.89) which is 106.96 % and 30.34 % higher respectively than no sulphur application to both the crops.