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Accelerating land-use change (LUC) in the Nilgiri Hill Region (NHR) has caused its land to mortify. Although this deterioration has been documented, the destruction of buried gem soil has not been reported. Therefore, this study was conducted to assess the impact of LUC on soil-carbon dynamics in the six major ecosystems in the NHR: croplands (CLs), deciduous forests (DFs), evergreen forests (EFs), forest plantations (FPs), scrublands (SLs), and tea plantations (TPs). Sampling was conducted at selected sites of each ecosystem at three depth classes (0–15, 15–30, and 30–45 cm) to quantify the carbon pools (water-soluble carbon, water-soluble carbohydrates, microbial biomass carbon, microbial biomass nitrogen, dehydrogenase, and different fractions of particulate organic carbon). We found that the LUC significantly decreased the concentration of carbon in the altered ecosystems (49.44–78.38%), with the highest being recorded at EF (10.25%) and DF (7.15%). In addition, the effects of the LUC on the aggregate size of the organic carbon were dissimilar across all the aggregate sizes. The relatively high inputs of the aboveground plant residues and the richer fine-root biomass were accountable for the higher concentration of carbon pools in the untouched EFs and DFs compared to the SLs, FPs, TPs, and CLs. The results of the land-degradation Index (LDI) depicted the higher vulnerability of TP (−72.67) and CL (−79.00). Thus, our findings highlight the global importance of LUC to soil quality. Henceforth, the conservation of carbon pools in fragile ecosystems, such as the NHR, is crucial to keep soils alive and achieve land-degradation neutrality.