We report results of telescope polarimetric imaging of the Moon with a CCD LineScan Camera at large phase angles, near 88°. This allows measurements of the polarization degree with an absolute accuracy better than 0.3% and detection of features with polarization contrast as small as 0.1%. The measurements are carried out in two spectral bands centered near 0.65 and 0.42 μm. We suggest characterizing the lunar regolith with the parameter a(Pmax)A, where Pmax,A, and a are the degree of maximum polarization, albedo, and the parameter describing the linear regression of the correlation Pmax–A. The parameter bears significant information on the particle characteristic size and packing density of the lunar regolith. We also suggest characterizing the lunar regolith with color-ratio images obtained with a polarization filter at large phase angles. We here consider the color-ratios C||(0.65/0.42 μm) and C⊥(0.65/0.42 μm). Using light scattering model calculations we show that the color-ratio images obtained with a polarization filter at large phase angles suggest a new tool to study the lunar surface. In particular, it turns out that the color-ratios C||(0.65/0.42 μm) and C⊥(0.65/0.42 μm) are sensitive to somewhat different thicknesses of the surfaces of regolith particles. We consider the applicability of the Hubble Space Telescope, the Very Large Telescope (ESO), and a spacecraft on a lunar polar orbit for polarimetric observations of the lunar surface.