The radiative effect of anthropogenic aerosols over Europe during the 2008 European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions Long Range Experiment (EUCAARI-LONGREX) campaign has been calculated using measurements collected by the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 aircraft and radiative transfer modelling. The aircraft sampled anthropogenically perturbed air masses across north-western Europe under anticyclonic conditions with aerosol optical depths ranging from 0.047 to 0.357. For one specially designed “radiative closure” flight, simulated irradiances have been compared to radiation measurements for a case of aged European aerosol in order to explore the validity of model assumptions and the degree of radiative closure that can be attained given the spatial and temporal variability of the observations and their measurement uncertainties. Secondly, the diurnally averaged aerosol radiative effect throughout EUCAARI-LONGREX has been calculated. The surface radiative effect ranged between −3.9 and −22.8 W m⁻² (mean −11 ± 5 W m⁻²), whilst top-of-the-atmosphere (TOA) values were between −2.1 and −12.0 W m⁻² (mean −5 ± 3 W m⁻²). We have quantified the uncertainties in our calculations due to the way in which aerosols and other parameters are represented in a radiative transfer model. The largest uncertainty in the aerosol radiative effect at both the surface and the TOA comes from the spectral resolution of the information used in the radiative transfer model (∼ 17 %) and the aerosol description (composition and size distribution) used in the Mie calculations of the aerosol optical properties included in the radiative transfer model (∼ 7 %). The aerosol radiative effect at the TOA is also highly sensitive to the surface albedo (∼ 12 %).