Desertification, which affects more than two-thirds of the world's arid and semi-arid regions, is a significant global ecological and environmental problem. There is a strong link between desertification of the drylands and emission of CO₂ from soil and vegetation to the atmosphere. The Horqin Sandy Land is a severely desertified area in China's agro-pastoral ecotone due to its fragile ecology, combined with unsustainable land management. We estimated changes of organic carbon content in the bulk soil (0–5 cm), in the light-fraction of soil organic matter (based on density fractionation), and in the various particle-size fractions in areas with mobile sand dunes after implementing grazing exclusion (12 and 27 years) and tree and shrub planting (22 and 24 years). Carbon stocks in the bulk soil and all soil density and particle-size fractions increased significantly in the exclosure and plantation plots. The average rates of carbon accumulation in the bulk soil in the exclosure and plantation plots were 16.0 and 17.8 g m^-2 y^-1, respectively, versus corresponding values of 2.3 and 7.1 g m^-2 y^-1 for the light fraction, 4.3 and 8.0 g m^-2 y^-1 for the coarse fraction, 5.0 and 3.4 g m^-2 y^-1 for the fine sand, 4.5 and 4.2 g m^-2 y^-1 for the very fine sand, and 1.8 and 1.8 g m^-2 y^-1 for the silt clay fraction. The older the exclosure and plantation, the more carbon accumulated in the bulk soil and in each fraction. The carbon pool exceeded the level in non-desertified grasslands after 27 years of grazing exclosure and 24 years of the shrub plantation. Our results suggest that both grazing exclusion and planting trees and shrubs can restore desertified grassland, creating a high potential for sequestering soil carbon, but that the plantations appeared to accumulate soil carbon faster than the exclosures.