The Sung Valley ultramafic–alkaline–carbonatite complex (UACC) of Meghalaya, NE, India, is a result of magmatic activity related to the Kerguelen mantle plume spanning from 101 to 115 Ma. In the present study, an integrated crystal size distribution (CSD), mineral chemistry, and melt inclusion analysis are carried out on the ijolites present within this UACC. The CSD analysis shows that these ijolites were formed in multiple stages through changes in the crystallization environment, such as cooling and nucleation rates. Raman spectroscopy of mineral inclusions of rutile, aphthitalite, apatite, carbonate–silicate melt inclusions, and disordered graphite within clinopyroxene and titanite, respectively, indicates a heterogeneous composition of the parental magma. These mineral and melt inclusion phases further suggest localized changes in oxygen fugacity (fO2) due to redox reactions in the lower crust. SEM–EDX analysis of the exposed melt inclusions reveals the presence of alkali-bearing diopside, phlogopite, and andradite, along with an unidentified carbonated silicate daughter phase. The studied melt inclusions are dominated by carbonate, whereas silicates are subordinate. The presence of this fully crystallized carbonate–silicate melt as calcite, diopside, phlogopite, magnetite, apatite, and andradite suggests the presence of “nano-calciocarbonatites” in these ijolites. Our study provides insights into different mechanisms of the loss of alkalies from initially entrapped alkaline carbonate melt in clinopyroxenes. The predominant occurrence of calcite as the only carbonate phase in the studied melt inclusions is a result of silicate–carbonate melt immiscibility, calcite-normative system in these inclusions, dealkalization of the alkaline carbonates in the presence of external fluid, and/or redistribution of the alkalies to the daughter alkali-bearing silicates.