Based on the optimal estimation (OE) theory, an inversion framework for aerosol retrieval from multiviewing polarimetric satellite measurements, is presented. The retrieved parameters include the wavelength-independent volume concentration and spectral aerosol optical depth (AOD). An OE-iteration approach is proposed to implement the framework. Polarization data from the polarization and directionality of the Earth’s reflectance sensor over the Chinese Beijing–Tianjin–Hebei region are selected to test the proposed algorithm. The validation against aerosol robotic network products produces high correlation coefficients (R) of 0.85, 0.9, and 0.86 for the fine-mode volume concentration, fine-mode AOD, and total AOD at 500 nm, respectively. These results indicate that the OE retrieval framework is practical and useful in the quantitative retrieval of AOD and fine-mode volume concentration from the multiangle polarization data.