Carbon dioxide (CO2) is one of the most important anthropogenic greenhouse gases (GHG) and significantly affects the energy balance of atmospheric systems. Larger coverage and higher spatial resolution of CO2 measurements can complement the existing in situ network and satellite measurements and thus improve our understanding of the global carbon cycle. In this study, we present a self-made airborne infrared remote sensing spectrometer (Air-IRSS) designed to determine the regional distribution of CO2. The Air-IRSS measured CO2 in the spectral range between 1590 and 1620 nm at a spectral resolution of 0.45 nm and an exposure time of 1 s. It was operated onboard an aircraft at a height of 3 km with a velocity of 180 km/h, and a spatial resolution of 50.00 m × 62.80 m. Weighting function modified differential optical absorption spectroscopy (WFM-DOAS) was used to analyze the measured spectra. The results show that the total uncertainty estimated for the retrieval of the CO2 column was 1.26% for airborne measurements over a large region, and 0.30% for a fixed point, such as power points or factories. Under vibration-free static conditions, the on-ground Air-IRSS observations can adequately reproduce the variations observed by Greenhouse Gases Observing Satellite (GOSAT )with a correlation coefficient (r) of 0.72. Finally, we conducted an airborne field campaign to determine the regional distribution of CO2 over the North China Plain. The regional distribution of CO2 columns over four cities of Xing-tai, Hengshui, Shijiazhuang, and Baoding were obtained with the GPS information, which ranged from 2.00 × 1021 molec cm-2 to 3.00 × 1021 molec cm-2. The CO2 vertical distributions were almost uniform below a height of 3 km in the area without CO2 emission sources, and the highest values were found over Baoding City.