The determination of aerosol direct radiative forcing over desert regions requires accurate information about the aerosol single-scattering albedo (SSA); however, the brightness of desert surfaces in the visible and near-IR range complicates the retrieval of aerosol optical properties using passive space-based measurements. Here we use the critical reflectance method to retrieve spectral aerosol absorption from space over North Africa, a desert region that is predominantly impacted by absorbing dust and biomass burning aerosol. We examine the sensitivity of the critical reflectance parameter to aerosol physical and optical properties that are representative of the region, and we find that the critical reflectance has low sensitivity to assumptions of aerosol size and refractive index for dust-like particles, except at scattering angles near 180°, which should be avoided with this method. We use our findings to retrieve spectral SSA from critical reflectance derived from Moderate Resolution Imaging Spectroradiometer (MODIS) reflectances in the vicinity of two Aerosol Robotic Network (AERONET) stations: Tamanrasset, in the Algerian Sahara, and Banizoumbou, in the Sahel. We retrieve lower aerosol SSAs at Banizoumbou, which is often impacted by dust-smoke mixtures, and higher SSAs at Tamanrasset, where pure desert dust is the dominant aerosol. Our results generally fall within the AERONET uncertainty envelopes, although at Banizoumbou we retrieve a spectral dependence different from that of AERONET. On the basis of our analysis, we expect to be able to retrieve SSA from critical reflectance for pure dust with an uncertainty of 0.02 and to provide spatial and spectral SSA information that will help reduce current uncertainties in the aerosol radiative forcing over desert regions.