The Grain for Green Programme (GGP) was launched in China in 1999 to control erosion and increase vegetation cover. Budgeted at USD 40 billion, GGP has converted over 20 million hectares of cropland and barren land into primarily tree-based plantations. Although GGP includes energy forests, only a negligible part (0.6%) is planted as such, most of the land (78%) being converted for protection. Future use of these plantations is unclear and an energy substitution hypothesis is valid. We estimate the overall carbon sequestration via GGP using official statistics and three approaches, based on i) net primary production, ii) IPCC's greenhouse gas inventory guidelines, and iii) mean annual increment. We highlight uncertainties associated with GGP and the estimates. Results indicate that crop- and barren-land conversion sequestered 222-468 Mt of carbon over GGP's first ten years, the IPCC approach yielding the highest estimate and the other two approaches yielding similar but lower estimates (approximately 250 Mt of carbon). The carbon stock in these plantation systems yields a mean of 12.3 t of carbon per hectare. Assessment uncertainties concern the use of growth curves not designed for particular species and locations, actual plantation survival rates, and discrepancies in GGP figures (e.g., area, type, and survival rate) at different authority levels (from national to local). The carbon sequestered in above- and below-ground biomass from GGP represents 14% (based on the median of the three approaches) of China's yearly (2009) carbon dioxide emissions from fossil fuel use and cement production.