Abstract. Accurate knowledge of the reflectance from snow/ice-covered surfaces is of fundamental importance for the retrieval of snow parameters and atmospheric constituents from space-based and airborne observations. In this paper, we simulate the reflectance in a snow–atmosphere system, using the phenomenological radiative transfer model SCIATRAN, and compare the results with that of airborne measurements. To minimize the differences between measurements and simulation, we determine and employ the key atmospheric and surface parameters, such as snow grain morphologies (or habits). First, we report on a sensitivity study. This addresses the requirement for adequate a priori knowledge about snow models and ancillary information about the atmosphere. For this aim, we use the well-validated phenomenological radiative transfer model, SCIATRAN. Second, we present and apply a two-stage snow grain morphology (i.e., size and shape of ice crystals in the snow) retrieval algorithm. We then describe the use of this new retrieval for estimating the most representative snow model, using different types of snow morphologies, for the airborne observation conditions performed by NASA's Cloud Absorption Radiometer (CAR). Third, we present a comprehensive comparison of the simulated reflectance (using retrieved snow grain size and shape and independent atmospheric data) with that from airborne CAR measurements in the visible (0.670 µm) and near infrared (NIR; 0.870 and 1.6 µm) wavelength range. The results of this comparison are used to assess the quality and accuracy of the radiative transfer model in the simulation of the reflectance in a coupled snow–atmosphere system. Assuming that the snow layer consists of ice crystals with aggregates of eight column ice habit and having an effective radius of ∼99 µm, we find that, for a surface covered by old snow, the Pearson correlation coefficient, R, between measurements and simulations is 0.98 (R2∼0.96). For freshly fallen snow, assuming that the snow layer consists of the aggregate of five plates ice habit with an effective radius of ∼83 µm and having surface inhomogeneity, the correlation is ∼0.97 (R2∼0.94) in the infrared and 0.88 (R2∼0.77) in the visible wavelengths. The largest differences between simulated and measured values are observed in the glint area (i.e., in the angular regions of specular and near-specular reflection), with relative azimuth angles <±40∘ in the forward-scattering direction. The absolute difference between the modeled results and measurements in off-glint regions, with a viewing zenith angle of less than 50∘, is generally small ∼±0.025 and does not exceed ±0.05. These results will help to improve the calculation of snow surface reflectance and relevant assumptions in the snow–atmosphere system algorithms (e.g., aerosol optical thickness retrieval algorithms in the polar regions).