Carbonate–silicate liquid immiscibility is the most widely accepted petrogenetic model for explaining the origin of carbonatites, accounting for approximately three-quarters of global carbonatite occurrences. Many, however, attribute the coexistence of carbonatites and alkaline silicate rocks to the coincidental emplacement of two independent parental magmas through a single crustal conduit. Thus, the exact cause of the carbonatite-alkaline silicate rock association remains equivocal. Here, we present the results of 40Ar/39Ar dating, geochemical, and C-O-Sr–Nd-Pb isotopic investigations of the Sarnu-Dandali carbonatite-alkaline complex, part of the Deccan Large Igneous Province (LIP), to shed light on this coexistence. Additionally, we explore the roles of the Deccan-Reunion mantle plume and the Indian continental lithosphere in generating the carbonatites of the complex. 40Ar/39Ar age data reveal that, although the complex underwent multiple cycles of alkaline magmatism, the activity at ~ 68.8 Ma was synchronous with the carbonatite intrusion. Interlaced spatial association of carbonatites and alkaline silicate rocks, including melt inclusions of the former in the latter, their complementary trace element patterns (and δ13C and δ18O), and overlapping initial Sr–Nd-Pb isotopic ratios indicate their co-genesis through carbonate–silicate liquid immiscibility. Trace element and isotopic ratio modeling suggests that the parental melanephelinitic magma for the complex evolved through concurrent crustal assimilation (up to 6%), fractional crystallization of silicates, and immiscible separation of carbonate melt, with the latter occurring before phonolite crystallization. The least contaminated isotopic ratios suggest that the parental carbonated-silicate magma derived from a mantle source with a mixed signature of the Reunion plume and metasomatized continental lithosphere.