To aid the understanding of how urbanisation has influenced anthropogenic CO2 and air pollutant emissions across all world regions, we make use of the latest developments of the Emissions Database for Global Atmospheric Research. In this study, we systematically analyse over 5 decades of emissions from different types of human settlements (from urban centres to rural areas) for different sectors in all countries. Our analysis shows that by 2015, urban centres were the source of a third of global anthropogenic greenhouse gases and most of the air pollutant emissions. The high levels of both population and emissions in urban centres therefore call for focused urban mitigation efforts.