To explore the atmospheric emissions of coal-fired power sector in China, a unit-based method was developed based on detailed information of unit type, fuel quality, emission control technology, and geographical location. During 2000–2005, the period when power sector developed fastest in the past 20 years, SO2, NOx and PM emissions of coal-fired power plants increased by 1.5, 1.7 and 1.2 times, respectively. The SO2 emission of coal-fired power sector was estimated to be 16097 kt in 2005, and would decrease to 11801 kt in 2010, attributed mainly to the wide application of the flue gas desulfurization (FGD) technology. The NOx emission, however, would increase from 6965 kt in 2005 to 9680 kt in 2010, since few NOx control measures would be taken during the five years. The TSP, PM, and PM emissions in 2005 were estimated to be 2774, 1842 and 994 kt, and the values would be 2540, 1824 and 1090 kt in 2010 respectively. The wet FGD would play an important role on dust emission removal. Through faithful implementation of closing small units and emission control policies in the acid rain and sulfur dioxide control zones, approximately 33%, 6% and 25% of SO2, NOx, and TSP emissions respectively could be further reduced in 2010. Emissions in 2015 and 2020 of coal-fired power plants were predicted applying scenario analysis. For SO2 and TSP, optimistic situation can be achieved through reasonable control policies; in contrast, NOx would probably be a more serious issue in future.