Single scattering albedo (SSA) governs the strength of aerosols in absorbing solar radiation, but few methods are available to directly measure this important quantity. There currently exist many ground-based measurements of spectral transmittance from which aerosol optical thickness (AOT) are retrieved under clear sky conditions. Reflected radiances at the top of the atmosphere as measured by a spaceborne spectroradiometer are sensitive to both AOT and SSA. On the basis of extensive radiative transfer simulations, it is demonstrated that the combined use of the two measurements allows for the retrieval of SSA at a reasonable accuracy under moderate to heavy aerosol loadings. Retrieval of SSA is most sensitive to AOT and surface reflectance.