Restoring disturbed and over-exploited ecosystems is important to mitigate human pressures on natural ecosystems. China has launched an ambitious national ecosystem restoration program called Grain to Green Program (GTGP) over the last decade. By using remote sensing techniques and ecosystem modelling, we quantitatively evaluated the changes in ecosystem carbon sequestration since China's GTGP program during period of 2000-2008. It was found the NPP and NEP in this region had steadily increased after the initiative of the GTGP program, and a total of 96.1 Tg of additional carbon had been sequestered during that period. Changes in soil carbon storage were lagged behind and thus insignificant over the period, but was expected to follow in the coming decades. As a result, the Loess Plateau ecosystem had shifted from a net carbon source in 2000 to a net carbon sink in 2008. The carbon sequestration efficiency was constrained by precipitation, and appropriate choices of restoration types (trees, shrubs, and grasses) in accordance to local climate are critical for achieving the best benefit/cost efficiency.