Low cost sensors are becoming increasingly available for studying urban air quality. Here we show how such sensors, deployed as a network, provide unprecedented insights into the patterns of pollutant emissions, in this case at London Heathrow Airport (LHR). Measurements from the sensor network were used to unequivocally distinguish airport emissions from long range transport, and then to infer emission indices from the various airport activities. These were used to constrain an air quality model (ADMS-Airport), creating a powerful predictive tool for modelling pollutant concentrations. For nitrogen dioxide (NO2), the results show that the non-airport component is the dominant fraction (∼75%) of annual NO2 around the airport and that despite a predicted increase in airport related NO2 with an additional runway, improvements in road traffic fleet emissions are likely to more than offset this increase. This work focusses on London Heathrow Airport, but the sensor network approach we demonstrate has general applicability for a wide range of environmental monitoring studies and air pollution interventions.