Investigating concentrations and spatial patterns of physicochemical parameters in landfill leachate and their profound impacts on stream sediments is an important issue for environmental sustainability. Therefore, the present study showed that the specifics landfill leachate and its interactions with stream sediments within the unique geological context of semi-arid basaltic terrain of the Deccan Volcanic Province in Pune, India. Employing advanced geo-accumulation indices and crystal phase differentiation methods, the study unveils the intricate metamorphosis of heavy metals and mineralogical composition, tracing the transformative journey from leachate to sediments. Noteworthy revelations emerge, particularly in the striking associations between heavy metals and the mineralogical composition, which encompasses primary and secondary minerals (calcite, quartz, and Fe–Mg oxides). These findings underscore the acceleration of weathering processes within this distinctive geological milieu. The 'geo-accumulation index' exhibits pronounced elevations in proximity to the landfill site, with persistence downstream, reliant upon the evolving weathering and accumulation dynamics. The lower reaches of the study area have higher concentrations of various heavy metals (Fe, Mn, Zn, Cr, Cu, Ni, Co, Hg, As, and Cd). These heavy metals are primarily sequestered within silt-dominated sediments conquered by augite, olivine and plagioclase minerals. Present research reveals the complex interplay between heavy metals in leachate and their physical and chemical interactions with sedimentary materials. These gradational shifts in mineralogy and geochemistry serve as compelling evidence of the transformative impact of leachate discharge within the distinctive basaltic geological framework. This study offers valuable insights into the complex environmental processes occurring at the intersection of landfill leachate and natural geological formations, enhancing the understanding of the dynamic geochemical interactions that shape this semi-arid basaltic terrain.