In early 2020 from April to early June, the metropolitan area of Sydney as well as the rest of New South Wales (NSW, Australia) experienced a period of lockdown to prevent the spread of COVID-19 virus in the community. The effect of reducing anthropogenic activities including transportation had an impact on the urban environment in terms of air quality which is shown to have improved for a number of pollutants, such as Nitrogen Dioxides (NO2) and Carbon Monoxide (CO), based on monitoring data on the ground and from a satellite. In addition to primary pollutants CO and NOx emitted from mobile sources, PM2.5 (primary and secondary) and secondary Ozone (O3) during the lockdown period will also be analyzed using both statistical methods on air quality data and the modelling method with emission and meteorological data input to an air quality model. By estimating the decrease in traffic volume in the Sydney region, the corresponding decrease in emission input to the Weather Research and Forecasting—Community Multiscale Air Quality Modelling System (WRF-CMAQ) air quality model is then used to estimate the effect of lockdown on the air quality especially CO, NO2, O3, and PM2.5 in the Greater Metropolitan Region (GMR) of Sydney. The results from both statistical and modelling methods show that NO2, CO, and PM2.5 levels decreased during the lockdown, but O3 instead increased. However, the change in the concentration levels are small considering the large reduction of ~30% in traffic volume.