We present an analysis of Titan data acquired by the Cassini Visual and Infrared Mapping Spectrometer (VIMS), making use of recent improvements in methane spectroscopic parameters in the region 1.3-5.2 μm. We first analyzed VIMS spectra covering a 8 × 10-km2 area near the Huygens landing site in order to constrain the single scattering albedo (ω0) of the aerosols over all of the VIMS spectral range. Our aerosol model agrees with that derived from Huygens Probe Descent Imager/Spectral Radiometer (DISR) in situ measurements below 1.6 μm. At longer wavelengths, ω0 steadily decreases from 0.92 at 1.6 μm to about 0.70 at 2.5 μm and abruptly drops to about 0.50 near 2.6 μm, a spectral variation that differs from that of Khare et al.'s (Khare, B.N., Sagan, C., Arakawa, E.T., Suits, F., Callcott, T.A., Williams, M.W. [1984]. Icarus 60, 127-137) laboratory tholins. Our analysis shows that the far wings of the strong methane bands on both sides of the transparency windows provide a significant source of opacity in these windows, and that their unknown sub-Lorentzian behavior limits our ability to determine precisely the surface albedos. Below 1.6 μm, the retrieved surface albedos agree with those derived from Huygens/DISR. The VIMS spectrum at 2.0 μm indicates a surface albedo of 0.11 ± 0.01, larger than derived in previous studies, and inconsistent with the signature of water ice. A series of VIMS data taken from 2004 to 2010 between 40°S and 40°N were then analyzed to monitor the latitudinal and temporal evolution of the atmospheric aerosol content. In the 2004-2008 period, the haze extinction is larger at Northern mid-latitudes by ˜20% with respect to the Huygens site, whereas Southern mid-latitudes are depleted by ˜15-20%. In 2009-2010, a progressive decline of the haze content in the Northern hemisphere is observed but no reversal of the North-to-South asymmetry is seen till mid-2010. Finally, data from five regions in Tui Regio and Fensal that show markedly different spectral behaviors and morphologies were analyzed to investigate the wavelength dependence of their surface albedo. The difference between bright and dark regions can be explained by different contents of small-sized tholins at the surface, brighter regions being more tholin-rich than dark regions, including the Huygens landing site. On the other hand, the albedo spectrum of the so-called blue regions, either dark or bright, can be explained by an excess of water ice particles, compared with the Huygens landing site. The spectrum of a 5-μm bright region in Tui Regio indicates a large excess of small-sized tholins relative to the Huygens site, but does not point to any particular surface composition.