The dataset contains air quality (VOCs) and GHGs (CO2, N2O, CH4, SF6) data at different height profiles collected in the frame of the ICARUS aerial campaigns. The aircraft operated at different height profiles above three European cities (Athens, Thessaloniki and Ljubljana) over sites with different characteristics (urban, suburban, rural) providing measurements of air pollutants and GHGs concentrations using sensor technologies as well as special sampling instrumentation. The data are stored in a single MS-Excel file named “Aerial_campaign_data.xlsx” which encompasses two worksheets: one named “Airplane_GHGs” which includes GHGs concentration levels measured over the 3 cities and the second named “Airplane_VOC's_Conc” which includes VOCs (benzene, toluene, o – Xylene, and m,p – Xylenes) concentrations measured over the 3 cities. Data are reported as average concentrations respectively above and below the atmospheric mixing layer.