The inversion precision of atmospheric aerosol parameters can be more effectively improved by the combination of multi-angle polarization and radiation data, so the airborne experiment is designed and completed to obtain multi-angle polarization and radiation data. The self-developed multi-angle directional polarized camera (DPC) is equipped on the aircraft, and sun-photometer CE318 is mounted at ground stations, then aviation flight experiment was carried out by designing aircraft’s course series ground stations. The data obtained from airborne experiment is analyzed, and the results show that DPC on the aircraft can obtain high precision polarization and radiation data. The atmospheric aerosols optical depth is retrieved using the experiment data, and inversion error is less than 3%, which demonstrates validity of multi-angle polarization and radiation data from airborne experiment.