China is the largest contributor to global atmospheric mercury (Hg), and accurate emission inventories in China are needed to reduce large gaps existing in global Hg mass balance estimates and assess Hg effects on various ecosystems. The China Atmospheric Mercury Emission (CAME) model was developed in this study using probabilistic emission factors generated from abundant on-site measurements and literature data. Using this model, total anthropogenic Hg emissions were estimated to be continuously increasing from 356 t in 2000 to 538 t in 2010 with an average annual increase rate of 4.2%. Industrial coal combustion, coal-fired power plants, nonferrous metal smelting, and cement production were identified to be the dominant Hg emission sources in China. The ten largest contributing provinces accounted for nearly 60% of the total Hg emissions in 2010. Speciated Hg emission inventory was developed over China with a grid-resolution of 36 × 36 km, providing needed emission fields for Hg transport models. In this new inventory, the sectoral Hg speciation profiles were significantly improved based on the latest data from field measurements and more detailed technology categorization. The overall uncertainties of the newly developed inventory were estimated to be in the range of -20% to +23%.