Since 2007, more than half of the world's population live in urban areas. Megacities, urban agglomerations with more than 10 million inhabitants, are rapidly increasing in number: in 1950 there were only two, New York and Tokyo with ~12 million, while by 2005 there were already 20, with Tokyo ranging the 35 millions. The urban atmospheres of these megacities are dominated by pollutants associated with vehicular emissions, as well as the formation of secondary pollutants responsible for photochemical smog. A comparative assessment of emissions and concentrations of volatile organic compounds (VOC) and carbon monoxide (CO) ratios in London (L) and Paris (P) is hereby presented. The work is based on three recent studies by Baker et al. (2008), Parrish et al. (2009) and von Schneidemesser et al. (in press) where concentrations of these compounds were analyzed for 28 US cities in the former and some global megacities in the second and third studies. Considering the fact that VOC provide information on the main emissions sources of cities, these studies found that even though concentrations of VOC varied greatly among cities, the ratio with the combustion tracer CO remained rather constant and was very useful for city comparison, as well as a good indicator of traffic emissions. VOC patterns in ambient air concentrations were observed to be similar in most cities, being able to consider that deviations from those patterns could be the result of measurement problems. Nevertheless, the representation of these emissions in global inventories has large uncertainties. The goal of our study is to compare and contrast emission inventory estimates with measured ambient concentrations of non-methane hydrocarbons (NMHC) and CO, as well as NMHC:CO ratios. Within the European CityZen project we have built an updated global emissions inventory with the best available datasets of anthropogenic, biomass burning and natural sources. As part of this research we will follow the same approach to compare emissions ratios between NMHC and CO for the megacities region of Paris and London and to compare these trends with measured ambient concentrations from three monitoring sites: Eltham (L) suburban station, Marylebone Road (L) kerbside station and Les Halles (P) urban station for the period 1997-2006.