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Retrieval of complete aerosol properties over land through remote sensing requires accurate information about the polarization characteristics of natural land surfaces. In this paper, a new bidirectional polarization distribution function (BPDF) is proposed, using the generalized regression neural network (GRNN). This GRNN-based BPDF model builds a quite accurate nonlinear relationship between polarized reflectance and four input parameters, i.e., Fresnel factor, scattering angle, red, and near-infrared reflectances. It learns fast because only a smoothing parameter needs to be adjusted. The GRNN-based model is compared to six widely used BPDF models (i.e., Nadal−Bréon, Maignan, Waquet, Litivinov, Diner, and Xie−Cheng models), using the Polarization and Directionality of the Earth’s Reflectance (POLDER) measurements. Experiments suggest that the GRNN-based BPDF model is more accurate than these models. Compared with the best current models, the averaged root-mean-square error (RMSE) from the GRNN-based BPDF model can be reduced by 13.4% by using data collected during the whole year and is lower for 97.4% cases with data collected during every month. Moreover, compared to the widely used BPDF models, the GRNN-based BPDF model provides better performance when the scattering angle is small, and it is the first model that is able to reproduce negative polarized reflectance. The GRNN-based BPDF model is thus useful for the remote sensing of complete aerosol properties over land.