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The Directional Polarimetric Camera (DPC) carried by the Chinese GaoFen-5-02 (GF-5-02) satellite has the ability for multiangle, multispectral, and polarization detection and will play an important role in the inversion of atmospheric aerosol and cloud characteristics. To ensure the validity of the DPC on-orbit multiangle and multispectral polarization data, high-precision image registration and geolocation are vital. High-precision geometric model parameters are a prerequisite for on-orbit image registration and geolocation. Therefore, on the basis of the multiangle imaging characteristics of DPC, an on-orbit autonomous geometric calibration method without ground reference data is proposed. The method includes three steps: (1) preprocessing the original image of the DPC and the satellite attitude and orbit parameters; (2) scale-invariant feature transform (SIFT) algorithm to match homologous points between multiangle images; (3) optimization of geometric model parameters on-orbit using least square theory. To verify the effectiveness of the on-orbit autonomous geometric calibration method, the image registration performance and relative geolocation accuracy before and after DPC on-orbit geometric calibration were evaluated and analyzed using the SIFT algorithm and the coastline crossing method (CCM). The results show that the on-orbit autonomous geometric calibration effectively improves the DPC image registration and relative geolocation accuracy. After on-orbit calibration, the multiangle image registration accuracy is better than 1.530 km, the multispectral image registration accuracy is better than 0.650 km, and the relative geolocation accuracy is better than 1.275 km, all reaching the subpixel level (<1.7 km). [ABSTRACT FROM AUTHOR]