A model coupling a meteorological predictive model and a vegetation photosynthesis and respiration model was used to simulate CO2 concentrations over coastal basin areas, and modeling results were estimated with aircraft observations during a massive sampling campaign. Along with the flight tracks, the model captured the meteorological variables of potential temperature and wind speed with mean bias results of 0.8℃, and 0.2 m/s, respectively. These results were statistically robust, which allowed for further estimation of the model’s performance for CO2 simulations. Two high-resolution emission data sets were adopted to determine CO2 concentrations, and the results show that the model underestimated by 1.8 ppm and 0.9 ppm at higher altitude over the study areas during daytime and nighttime, respectively, on average. Overall, it was concluded that the model’s CO2 performance was fairly good at higher altitude over the study areas during the study period.