A spatially, temporally and chemically resolved emission inventory for particulate matter and gaseous species from anthropogenic and natural sources was created for the Greater Athens Area (GAA; base year, 2007). Anthropogenic sources considered in this study include combustion (industrial, non-industrial, commercial and residential), industrial production, transportation, agriculture, waste treatment and solvent use. The annual gaseous pollutants (ΝΟx, SOx, nonmethane volatile organic compounds (NMVOCs), CO and ΝΗ 3 ) and particulate matter (PM 2.5 and PM 2.5-10 ) emissions were derived from the UNECE/EMEP database for most source sectors (SNAP 1-9; 50× 50 km 2 ) and their spatial resolution was increased using surrogate spatial datasets (land cover, population density, location and emissions of large point sources, emission weighting factors for the GAA; 1×1 km 2 ). The emissions were then temporally disaggregated in order to provide hourly emissions for atmospheric pollution modelling using monthly, daily and hourly disintegration coefficients, and additionally the chemical speciation of size-segregated particles and NMVOCs emissions was performed. Emissions from agriculture (SNAP 10) and natural emissions of particulate matter from the soil (by wind erosion) and the sea surface and of biogenic gaseous pollutants from vegetation were also estimated. During 2007 the anthropogenic emissions of CO, SOx, NOx, NMVOCs, NH 3 , PM 2.5 and PM 2.5-10 from the GAA were 151,150, 57,086, 68,008, 38,270, 2,219, 9,026 and 3,896 Mg, respectively. It was found that road transport was the major source for CO (73.3%), NMVOCs (31.6%) and NOx (35.3%) emissions in the area. Another important source for NOx emissions was other mobile sources and machinery (23.1%). Combustion for energy production and transformation industries was the major source for SOx (38.5%), industrial combustion for anthropogenic PM 2.5-10 emissions (59.5%), whereas non-industrial combustion was the major source of PM 2.5 emissions (49.6%). Agriculture was the primary NH 3 source in the area (72.1%). Natural vegetation was found to be an important source of VOCs in the area which accounted for approximately the 5% of total VOCs emitted from GAA on a typical winter day. The contribution of seasalt particles to the emissions of PM 2.5 was rather small, whereas the emissions of resuspended dust particles exceeded by far the emissions of PM 2.5 and PM 2.5-10 from all anthropogenic sources.