Ozone and fine particles (PM_2.5) are the two main air pollutants of concern in the New South Wales Greater Metropolitan Region (NSW GMR) region due to their contribution to poor air quality days in the region. This paper focuses on source contributions to ambient ozone concentrations for different parts of the NSW GMR, based on source emissions across the greater Sydney region. The observation-based Integrated Empirical Rate Model (IER) was applied to delineate the different regions within the GMR based on the photochemical smog profile of each region. Ozone source contribution is then modelled using the CCAM-CTM (Cubic Conformal Atmospheric Model-Chemical Transport Model) modelling system and the latest air emission inventory for the greater Sydney region. Source contributions to ozone varied between regions, and also varied depending on the air quality metric applied (e.g., average or maximum ozone). Biogenic volatile organic compound (VOC) emissions were found to contribute significantly to median and maximum ozone concentration in North West Sydney during summer. After commercial domestic, power station was found to be the next largest anthropogenic source of maximum ozone concentrations in North West Sydney. However, in South West Sydney, beside commercial and domestic sources, on-road vehicles were predicted to be the most significant contributor to maximum ozone levels, followed by biogenic sources and power stations. The results provide information which policy makers can devise various options to control ozone levels in different parts of the NSW Greater Metropolitan Region.