Dust storms have large impacts on air quality and meteorological elements; however, their relationships with atmospheric greenhouse gases (e.g., CO2) and radiation components remain uncertain. In this study, the co-variation of dust and CO2 concentrations and its possible influencing mechanism are examined using observations at the Shangdianzi (SDZ) regional Global Atmosphere Watch (GAW) station along with simulations of the Vegetation Photosynthesis and Respiration Model coupled with the Weather Research and Forecasting model (WRF-VPRM), during two dust storm events on 15 and 28 March 2021. During these events, hourly CO2 concentrations decreased by 40–50 ppm at SDZ while dust concentrations increased to 1240.6 and 712.4 µg m−3. The elevated dust increased diffusive shortwave irradiance by 50–60% and decreased direct shortwave irradiance by ~60% along with clouds. The dust events were attributed to the passages of two cold front systems over northern China. At SDZ, during the frontal passages, wind speed increased by 3–6 m s−1, and relative humidity decreased by 50–60%. The CO2 variations associated with the frontal systems were captured by the WRF-VPRM despite the overestimated surface CO2 level at SDZ. Biogenic CO2 flux plays an indistinctive role in the large CO2 variation at SDZ, as it is weak during the non-growing season. The cold fronts pushed polluted air southeastward over the North China Plain and replaced it with low-CO2 air from Northwest China, leading to the decline in CO2. These findings demonstrate that mesoscale synoptic conditions significantly affect the regional transport and dispersion of CO2, which can influence the prediction of terrestrial carbon balance on a regional scale.