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The coupled Conformal Cubic Atmospheric Model (CCAM) and Chemical Transport Model (CTM) (CCAM-CTM) was undertaken with eleven emission scenarios segregated from the 2008 New South Wales Greater Metropolitan Region (NSW GMR) Air Emission Inventory to predict major source contributions to ambient PM2.5 and exposure in the NSW GMR. Model results illustrate that populated areas in the NSW GMR are characterised with annual average PM2.5 of 6–7 µg/m3, while natural sources including biogenic emissions, sea salt and wind-blown dust contribute 2–4 µg/m3 to it. Summer and winter regional average PM2.5 ranges from 5.2–6.1 µg/m3 and 3.7–7.7 µg/m3 across Sydney East, Sydney Northwest, Sydney Southwest, Illawarra and Newcastle regions. Secondary inorganic aerosols (particulate nitrate, sulphate and ammonium) and sodium account for up to 23% and 18% of total PM2.5 mass in both summer and winter. The increase in elemental carbon (EC) mass from summer to winter is found across all regions but particularly remarkable in the Sydney East region. Among human-made sources, "wood heaters" is the first or second major source contributing to total PM2.5 and EC mass across Sydney in winter. "On-road mobile vehicles" is the top contributor to EC mass across regions, and it also has significant contributions to total PM2.5 mass, particulate nitrate and sulphate mass in the Sydney East region. "Power stations" is identified to be the third major contributor to the summer total PM2.5 mass across regions, and the first or second contributor to sulphate and ammonium mass in both summer and winter. "Non-road diesel and marine" plays a relatively important role in EC mass across regions except Illawarra. "Industry" is identified to be the first or second major contributor to sulphate and ammonium mass, and the second or third major contributor to total PM2.5 mass across regions. By multiplying modelled predictions with Australian Bureau of Statistics 1-km resolution gridded population data, the natural and human-made sources are found to contribute 60% (3.55 µg/m3) and 40% (2.41 µg/m3) to the population-weighted annual average PM2.5 (5.96 µg/m3). Major source groups "wood heaters", "industry", "on-road motor vehicles", "power stations" and "non-road diesel and marine" accounts for 31%, 26%, 19%, 17% and 6% of the total human-made sources contribution, respectively. The results in this study enhance the quantitative understanding of major source contributions to ambient PM2.5 and its major chemical components. A greater understanding of the contribution of the major sources to PM2.5 exposures is the basis for air quality management interventions aiming to deliver improved public health outcomes. [ABSTRACT FROM AUTHOR]