We present an analysis of direct land use change (dLUC) resulting from the conversion of semiarid woodlands in Brazil and India to Jatropha curcas, a perennial biofuel crop. The sites examined include prosopis woodlands, managed for woodfuel production under periodic coppicing, in southern India, and unmanaged caatinga woodlands in the Brazilian state of Minas Gerais. The jatropha plantations under consideration include pruned and unpruned stands and ranged from 2 to 4 years of age. Stocks of carbon in aboveground (AG) pools, including woody biomass, coarse debris, leaf litter, and herbaceous matter, as well as soil organic carbon (SOC) were evaluated. The jatropha plantations store 8–10 tons of carbon per hectare (t C ha−1) in AG biomass and litter when managed with regular pruning in both India and Brazil. Unpruned trees, only examined in Brazil, store less biomass (and carbon), accumulating just 3 t C ha−1 in AG pools. The two woodlands that were replaced with jatropha show substantial differences in carbon pools: prosopis contains ∼11 t C ha−1 in AG stocks of carbon, which was very close to the jatropha stand which replaced it. In contrast, caatinga stores ∼35 t C ha−1 in AG biomass. Moreover, no change in SOC was detected in land that was converted from Prosopis to jatropha. As a result, there is no detectable change in AG carbon stocks at the sites in South India where jatropha replaced prosopis woodlands. In contrast, large losses of AG carbon were detected in Central Brazil where jatropha replaced native caatinga woodlands. These losses represent a carbon debt that would take 10–20 years to repay.