Atmospheric aerosol distributions from 2000 to 2007 are simulated with the Goddard Chemistry Aerosol Radiation and Transport (GOCART) model to attribute light absorption by aerosol to its composition and sources from pollution, dust, and biomass burning. The 8-year, global averaged total aerosol optical depth (τ ), absorption optical depth (τa ), and single scattering albedo (ω) at 550 nm are estimated at 0.14, 0.0086, and 0.95, respectively, with sulfate making the largest fraction of τ (37%), followed by dust (30%), sea salt (16%), organic matter (OM) (13%), and black carbon (BC) (4%). BC and dust account for 43% and 53% of τa , respectively. From a model experiment with “tagged” sources, natural aerosols are estimated to be 58% of τ and 53% of τa , with pollution and biomass burning aerosols to share the rest. Comparing with data from the surface sunphotometer network AERONET, the model tends to reproduce much better the AERONET direct measured data of τ and the Angström exponent (α) than its retrieved quantities of ω and τa . Relatively small in its systematic bias of τ for pollution and dust regions, the model tends to underestimate τ for biomass burning aerosols by 30–40%. The modeled α is 0.2–0.3 too low (particle too large) for pollution and dust aerosols but 0.2–0.3 too high (particle too small) for the biomass burning aerosols, indicating errors in particle size distributions in the model. Still, the model estimated ω is lower in dust regions and shows a much stronger wavelength dependence for biomass burning aerosols but a weaker one for pollution aerosols than those quantities from AERONET. These comparisons necessitate model improvements on aerosol size distributions, the refractive indices of dust and black carbon aerosols, and biomass burning emissions in order to better quantify the aerosol absorption in the atmosphere.