Airborne measurements of high-resolution spectral data are an innovative technology with high spatial resolution and informative features, and the high-resolution spectral data have high sensitivity of retrieving CO2 concentration near the surface of earth. The high-resolution atmospheric radiation software is used to calculate and choose the 1.57 μm (6315～6385 cm－1) waveband CO2 high-resolution spectra to retrieve CO2 concentration. The results show that the high-resolution spectral data can detect very small CO2 (1%) changes with sufficient signal to noise ratio and resolution. Also the effects of aerosols in atmospheric and surface temperature change on the high-resolution spectral data of CO2 are analyzed.