Mercury pollution control has become a global goal. The accurate estimate of long-term mercury emissions in China is critical to evaluate the global mercury budget and the emission reduction potentials. In this study, we used a technology-based approach to compile a consistent series of China's atmospheric mercury emissions at provincial level from 1978 to 2014. China totally emitted 13 294 t of anthropogenic mercury to air during 1978-2014, in which gaseous elemental mercury, gaseous oxidized mercury, and particulate-bound mercury accounted for 58.2%, 37.1%, and 4.7%, respectively. The mercury removed during this period were 2085 t in coal-fired power plants (counting 49% of mercury input), 7259 t in Zn smelting (79%), 771 t in coal-fired industrial boilers (25%), and 658 t in cement production plants (27%), respectively. Annual mercury emissions increased from 147 t in 1978 to 530 t in 2014. Both sectoral and spatial emissions of atmospheric mercury experienced significant changes. The largest mercury emission source evolved from coal-fired industrial boilers before 1998, to zinc smelting during 1999-2004, coal-fired power plants during 2005-2008, finally to cement production after 2009. Coal-fired industrial boilers and cement production have become critical hotpots for China's mercury pollution control.