The United Nations Environment Programme (UNEP) has begun a process of developing a legally binding instrument to manage emissions of mercury from anthropogenic sources. The UNEP Governing Council has concluded that there is sufficient evidence of significant global adverse impacts from mercury to warrant further international action; and that national, regional and global actions should be initiated as soon as possible to identify populations at risk and to reduce human generated releases. This paper describes the development of, and presents results from, a comprehensive, spatially and temporally resolved inventory of atmospheric mercury emissions from the Australian landmass. Results indicate that the best estimate of total anthropogenic emissions of mercury to the atmosphere in 2006 was 15 ± 5 tonnes. Three industrial sectors contribute substantially to Australian anthropogenic emissions: gold smelting (∼50%, essentially from a single site/operation), coal combustion in power plants (∼15%) and alumina production from bauxite (∼12%). A diverse range of other sectors contribute smaller proportions of the emitted mercury, but industrial emissions account for around 90% of total anthropogenic mercury emissions. The other sectors include other industrial sources (mining, smelting, and cement production) and the use of products containing mercury. It is difficult to determine historical trends in mercury emissions given the large uncertainties in the data. Estimates for natural and re-emitted emissions from soil, water, vegetation and fires are made using meteorological models, satellite observations of land cover and soil and vegetation type, fuel loading, fire scars and emission factors which account for the effects of temperature, insolation and other environmental variables. These natural and re-emitted sources comfortably exceed the anthropogenic emissions, and comprise 4–12 tonnes per year from vegetation, 70–210 tonnes per year from soils, and 21–63 tonnes per year from fires.