The Weather Research and Forecasting (WRF) model and Vegetation Photosynthesis and Respiration Model (VPRM) were coupled to simulate atmospheric CO2 concentrations. The performance of the WRF-VPRM to simulate regional scale CO2 concentration was estimated over coastal basin areas. Either Hestia 2011(HST) or Vulcan 2002(VUL) anthropogenic CO2 emission data were used in two numerical experiments for the study regions. Simulated meteorological variables were validated with ground and background CO2 measurement data, and the results show that the model captured temporal variations of CO2 concentration on a daily basis. CO2 directional analysis revealed that the dominant CO2 emission sources are located S and SW. The simulated Net Ecosystem Exchange (NEE) agreed relatively well with measured CO2 fluxes at each vegetation class site, showing approximately 40% at max improvement at shrub areas.