Numerical simulation and validation of three-dimensional structure of atmospheric carbon dioxide (CO<sub>2</sub>) is necessary for quantification of transport model uncertainty and its role on surface flux estimation by inverse modeling. Simulations of atmospheric CO<sub>2</sub> were performed using four transport models and two sets of surface fluxes compared with an aircraft measurement dataset of Comprehensive Observation Network for Trace gases by AIrLiner (CONTRAIL), covering various latitudes, longitudes, and heights. Under this transport model intercomparison project, spatiotemporal variations of CO<sub>2</sub> concentration for 2006–2007 were analyzed with a three-dimensional perspective. Results show that the models reasonably simulated vertical profiles and seasonal variations not only over northern latitude areas but also over the tropics and southern latitudes. From CONTRAIL measurements and model simulations, intrusion of northern CO<sub>2</sub> in to the Southern Hemisphere, through the upper troposphere, was confirmed. Furthermore, models well simulated the vertical propagation of seasonal variation in the northern free troposphere. However, significant model-observation discrepancies were found in Asian regions, which are attributable to uncertainty of the surface CO<sub>2</sub> flux data. In summer season, differences in latitudinal gradients by the fluxes are comparable to or greater than model-model differences even in the free troposphere. This result suggests that active summer vertical transport sufficiently ventilates flux signals up to the free troposphere and the models could use those for inferring surface CO<sub>2</sub> fluxes.