Yellow gypsum (YG), a synthetic gypsum derived from LD slag (steel industry by-product), is alkaline in nature and contains appreciable amounts of essential plant nutrients. Due to its chemical composition, YG has potential as a soil amendment to improve nutrient availability and reduce arsenic (As) mobility in contaminated soils. The present study evaluated the effectiveness of YG as a source of calcium (Ca), sulfur (S), silicon (Si) and iron (Fe) in kharif groundnut and boro-rice cropping systems grown in As-contaminated soil. A series of pot experiments was conducted during 2019–2021 using a factorial completely randomized design (FCRD) with 17 levels of As treatments and three levels of YG application (0, 30 and 60 kg ha-1). Irrespective of As treatments, the application of YG significantly (p < 0.05) increased the availability of S, Si and phosphorus (P), as well as exchangeable Ca and Diethylenetriaminepentaacetic acid (DTPA)-extractable Fe, across different growth stages of both crops. The YG application also resulted in a slight increase in soil pH. A significant (p < 0.05) increase in soil organic carbon (OC) was observed with YG application, whereas lower values were recorded in the control treatment (Y₀). Increasing As levels in soil were inversely related to the availability of Ca, S, Si and P, while no significant effect (p > 0.05) was observed on soil Fe and manganese (Mn) contents. Among the treatments, the application of gypsum (YG) at 60 kg ha-1 proved to be the most effective rate for improving soil nutrient availability in both crops under As- contaminated conditions. The results suggest that YG can serve as a beneficial soil amendment for enhancing soil fertility and managing nutrient dynamics and reducing the bioavailability of As in As-contaminated soils.