Green roofs are a promising approach to mitigate air pollution in urban environments, but limited experimental data is yet available. In this study, we developed a laboratory-scale setup to measure the removal nitrogen dioxide (NO2) and ozone (O3) using a variety of common green roof species. Experiments were conducted on detached leaves and whole plants using two chambers (0.6 L and 12 L), visible lighting, NOx/O3 sources and online analyzers. Three species were the best performant (Thymus vulgaris, Sedum sexangulare and Heuchera Americana L.) with deposition velocities (νd) ranging from 1.6 to 4.82 m/h for NO2, and 1.7–5.56 m/h for O3. In both cases, thyme was the most effective plant likely due to its higher stomatal area and the reactivity of its volatile metabolites with O3 leading to several oxidized by-products. Furthermore, NO2 uptake was found to be enhanced by surface water released by leaf transpiration leading to the production of nitrous acid (HONO). Similar values of (νd) were observed (3.84–4.65 m/h) when whole thyme plant was used. The soil was also found to be competitive in removing O3 but less performant in capturing NO2. Using a dry deposition model, we estimated that the three plant species can uptake up to 9 kg/ha/year of NO2 and 13.6 kg/ha/year, which fall in agreement with previously reported modeling data. Our experimental approach can be a rapid tool for screening the depollution performances of green roof species enabling an effective prioritization for deployment in urban environments.