Developing countries’ megacities, characterised by dense populations and socioeconomic disparities, often face high levels of pollutants, mainly from vehicle emissions. Poor air quality can lead to a range of public health problems which in turn, need to be addressed by public policies. The main goal of this article is to examine the impact of public policies and the influence of transport modes on air pollution of three districts from the Metropolitan Region of São Paulo, in Brazil: Pinheiros, Parque Dom Pedro II and Taboão da Serra. The method was held through a comparative analysis, which in turn, took into account urban indicators, urban mobility data and pollutants levels (CO and NOx). These data were collected from the 2007 and 2017 São Paulo Metrô Origin and Destination Surveys and the Air Quality Database of the Environmental Company of the State of São Paulo. As key findings, the three study areas’ pollutant concentrations presented a downward trend from 2007 to 2017 as the same time there was an increase in the public transport and non-motorized transport modes. However, it is important to highlight the confluence of the state and federal public policies occuring at the same period such as PRONCOVE, Rodoanel and the Yellow Subway Line. The identified socio-environmental disparities in the urban realm highlight the importance of localised analyses in order to reveal problems and opportunities to get a better response in terms of urban mobility and air quality. Thus, the perpetuation of constant policy’s updates and interdisciplinary collaboration is crucial.