Surface coal mining activities have numerous consequences on terrestrial ecosystems. Loss of soil and biomass carbon pool due to mining activities is a serious concern in the rapidly changing environment. We investigated the effect of fast-growing trees (Albizia lebbeck, Albizia procera, and Dalbergia sissoo) on soil fertility and ecosystem carbon pool after eight years of afforestation in the post-mining land of Jharia coalfield, India, and compared with the adjacent natural forest site. Significant differences in soil organic carbon (SOC) and total nitrogen (TN) stocks in afforested mine soil and natural forest soils were observed. Greater SOC stock was found under D. sissoo (30.17 Mg·C·ha−1) while total N stock was highest under A. lebbeck (4.16 Mg·N·ha−1) plantation. Plant biomass accumulated 85% of the natural forest carbon pool after eight years of afforestation. The study concluded that planting fast-growing trees in post-mining lands could produce a promising effect on mine soil fertility and greater carbon storage in a short period.