The atmospheric correction of optical remote sensing data requires the determination of aerosol and gas optical properties. A method is presented which allows the detection of the aerosol scattering effects from optical remote sensing data at spatial sampling intervals below 5 m in cloud-free situations from cast shadow pixels. The derived aerosol optical thickness distribution is used for improved atmospheric compensation. In a first step, a novel spectral cast shadow detection algorithm determines the shadow areas using spectral indices. Evaluation of the cast shadow masks shows an overall classification accuracy on an 80% level. Using the such derived shadow map, the ATCOR atmospheric compensation method is iteratively applied on the shadow areas in order to find the optimum aerosol amount. The aerosol optical thickness is found by analyzing the physical atmospheric correction of fully shaded pixels in comparison to directly illuminated areas. The shadow based aerosol optical thickness estimation method (SHAOT) is tested on airborne imaging spectroscopy data as well as on photogrammetric data. The accuracy of the reflectance values from atmospheric correction using the such derived aerosol optical thickness could be improved from 3–4% to a level of better than 2% in reflectance for the investigated test cases.