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 ( P max ) a A , where P max , A , and a are the degree of maximum polarization, albedo, and the parameter describing the linear regression of the correlation P max – 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.