Urban conurbations of East Africa are affected by harmful levels of air pollution. The paucity of local air quality networks and the absence of the capacity to forecast air quality make difficult to quantify the real level of air pollution in this area. The CHIMERE chemistry transport model has been used along with the Weather Research and Forecasting (WRF) meteorological model to run high-spatial-resolution (2 × 2 km) simulations of hourly concentrations of particulate matter with an aerodynamic diameter smaller than 2.5 µm (PM2.5) for three East African urban conurbations: Addis Ababa in Ethiopia, Nairobi in Kenya, and Kampala in Uganda. Two existing emission inventories were combined to test the performance of CHIMERE as an air quality model for a target monthly period in 2017, and the results were compared against observed data from urban, roadside, and rural sites. The results show that the model is able to reproduce hourly and daily temporal variabilities in aerosol concentrations that are close to observed values from urban, roadside, and rural environments. CHIMERE's performance as a tool for managing air quality was also assessed. The analysis demonstrated that, despite the absence of high-resolution data and up-to-date biogenic and anthropogenic emissions, the model was able to reproduce 66 %–99 % of the daily PM2.5 exceedances above the World Health Organization (WHO) 24 h mean PM2.5 guideline (25 µg m−3) in the three cities. An analysis of the 24 h average PM2.5 levels was also carried out for 17 constituencies in the vicinity of Nairobi. This showed that 47 % of the constituencies in the area exhibited a poor Air Quality Index for PM2.5 that was in the unhealthy category for human health, thereby exposing between 10 000 and 30 000 people per square kilometre to harmful levels of air contamination.