Surface albedo is an important forcing parameter that drives the radiative energy budget as it determines the fraction of the downwelling solar irradiance that the surface reflects. Here we report on ground-based measurements of the spectral albedo (350–2200 nm) carried out at 20 sites across a North–South transect of approximately 1300 km in the Atacama Desert, from latitude 18° S to latitude 30° S. These spectral measurements were used to evaluate remote sensing estimates of the albedo derived from the Moderate Resolution Imaging Spectroradiometer (MODIS). We found that the relative mean bias error (RMBE) of MODIS-derived estimates was within ± 5% of ground-based measurements in most of the Atacama Desert (18–27° S). Although the correlation between MODIS-derived estimates and ground-based measurements remained relatively high (R= 0.94), RMBE values were slightly larger in the southernmost part of the desert (27–30° S). Both MODIS-derived data and ground-based measurements show that the albedo at some bright spots in the Atacama Desert may be high enough (up to 0.25 in visible range) for considerably boosting the performance of bifacial photovoltaic technologies (6–12%).