Air pollution levels are generally believed to be higher in deprived areas but associations are complex especially between sensitive population subgroups. We explore air pollution inequalities at national, regional and city level in England and the Netherlands comparing particulate matter (PM10) and nitrogen dioxide (NO2) concentrations and publicly available population characteristics (deprivation, ethnicity, proportion of children and elderly). We saw higher concentrations in the most deprived 20% of neighbourhoods in England (1.5 μg/m(3) higher PM10 and 4.4 μg/m(3) NO2). Concentrations in both countries were higher in neighbourhoods with >20% non-White (England: 3.0 μg/m(3) higher PM10 and 10.1 μg/m(3) NO2; the Netherlands: 1.1 μg/m(3) higher PM10 and 4.5 μg/m(3) NO2) after adjustment for urbanisation and other variables. Associations for some areas differed from the national results. Air pollution inequalities were mainly an urban problem suggesting measures to reduce environmental air pollution inequality should include a focus on city transport.