In this paper, the amount of carbon sequestered through large-scale afforestation and related costs and benefits are calculated, assuming that the forests are managed in perpetual rotations. Based on land availability for afforestation, 20 cases are identified in five suitable regions in China. The least expensive way of developing forests for the purpose of sequestering carbon emissions is the case of Pinus massoniana from the initial investment point of view, and then Spruce. The cases of open forest management are relatively less expensive options because of their low initial investment and long rotations, although their annual wood increments are low. Some less productive tree species have higher net costs for carbon sequestering. For most of the agroforestry systems the net costs are low, especially in the south, the southwest, and the north of China, though their initial investments are high. If the total land available is afforested, the net carbon sequestering will be about 9.7 billion tons under perpetual rotations, amounting to 16.3 times the total industrial carbon release in 1988 in China, and the total initial cost for such a programme is estimated at 19.3 billion US$. Some hindrances in developing forests in China are discussed.