A coupled regional-to-local modelling system comprising a regional chemistry–climate model with 5 km horizontal resolution (EMEP4UK) and an urban dispersion and chemistry model with explicit road source emissions (ADMS-Urban) has been used to simulate air quality in 2012 across London. The study makes use of emission factors for NO x and NO 2 and non-exhaust emission rates of PM 10 and PM 2.5 which have been adjusted compared to standard factors to reflect real-world emissions, with increases in total emissions of around 30 % for these species. The performance of the coupled model and each of the two component models is assessed against measurements from background and near-road sites in London using a range of metrics concerning annual averages, high hourly average concentrations and diurnal cycles. The regional model shows good performance compared to measurements for background sites for these metrics, but under-predicts concentrations of all pollutants except O 3 at near-road sites due to the low resolution of input emissions and calculations. The coupled model shows good performance at both background and near-road sites, which is broadly comparable with that of the urban model that uses measured concentrations as regional background, except for PM 2.5 where the under-prediction of the regional model causes the coupled model to also under-predict concentrations. Using the coupled model, it is estimated that 13 % of the area of London exceeded the EU limit value of 40 µg m −3 for annual average NO 2 in 2012, whilst areas of exceedances of the annual average limit values of 40 and 25 µg m −3 for PM 10 and PM 2.5 respectively were negligible.