The versatile Generalized Retrieval of Aerosol and Surface Properties (GRASP) algorithm exploits the advantages of synergic ground-based aerosol observations such as radiometric (sensitive to columnar aerosol optical and microphysical properties) and lidar (sensitive to vertical distribution of the optical properties) observations. The synergy is possible when the complementary data is mutually constrained by GRASP parametrization that includes, for the first time ever, the degree of linear polarization (DoLP) parameter measured by a polarized sun-sky-lunar AERONET photometer (380, 440, 500, 675, 870, 1020, and 1640 nm) in synergy with the vertical profiles from an elastic lidar (355, 532, and 1064 nm). First, a series of numerical tests is performed using simulated data generated using a climatology of data and ground-based measurements. The inversions are performed with and without random noise for five different combinations of input data, starting from the AERONET-like dataset and increasing to the complex one by adding more information for three aerosol scenarios: I—high aerosol optical depth (AOD) with dominant coarse mode; II—low AOD with dominant coarse mode; III—high AOD with dominant fine mode. The inclusion of DoLP improves (i) the retrieval accuracy of the fine-mode properties when it is not dominant; (ii) the retrieval accuracy of the coarse-mode properties at longer wavelengths and that of the fine-mode properties at shorter wavelengths; (iii) the retrieval accuracy of the coarse-mode real part of the refractive index (up to 36% reduction), but has no effect on the retrieval of the imaginary part; (iv) reduces up to 83% the bias of the sphere fraction (SF) retrieval in coarse-mode dominated regimes; and (v) the root mean square error (RMSE) of the retrieval for most of the parameters in all scenarios. In addition, the addition of more photometer channels in synergy with a three-wavelength elastic lidar reduces the RMSE for the real part (67% in the coarse mode) and the imaginary part (35% in the fine mode) of the refractive index, the single scattering albedo (38% in the fine mode), the lidar ratio (20% in the coarse mode), and the SF (43%).