The use of reflective surfaces offers one low-cost solution for reducing solar loading to urban environments and the Earth that should be considered as part of sustainable urban design. Here, we characterize the radiative benefits, i.e. the additional shortwave radiation leaving the atmosphere, from the installation of highly reflective 'cool' roofs in urban areas in India that face relatively large local aerosol burdens. We use a previously tested column radiative transfer model to estimate the energy per unit area reflected to space from increasing the surface albedo at six cities within India. The model is used to characterize radiative transfer each day over five years (2008–2012) based on mid-day satellite retrievals of MODIS aerosol depth, cloud water path, and average surface albedo and MERRA atmospheric profiles of temperature and composition. Compared against ten months of field observations in two cities, the model derived incoming surface shortwave radiation estimates relative to observations show small biases (0.5% and −2.6%, at Pantnagar and Nainital, respectively). Despite the high levels of local aerosols we found cool roofs provided significant radiative benefits at all locations. Averaged over the five year period we found that increasing the albedo of 1 m2 of roof area by 0.5 would reflect to space 0.9–1.2 kWh daily from 08:30–15:30 LST, depending on location. This is equivalent to a constant forcing of 37–50 W m−2 (equivalent to reducing CO2 emissions by 74 to 101 kg CO2 m−2 roof area). Last, we identify a co-benefit of improving air quality, in that removing aerosols from the atmosphere could increase the radiative benefits from cool roofs by 23–74%, with the largest potential increase found at Delhi and the smallest change found at Nainital.