In this paper, an algorithm for the retrieval of aerosol and land surface properties from airborne spectropolarimetric measurements – combining neural networks and an iterative scheme based on Phillips–Tikhonov regularization – is described. The algorithm – which is an extension of a scheme previously designed for ground-based retrievals – is applied to measurements from the Research Scanning Polarimeter (RSP) on board the NASA ER-2 aircraft. A neural network, trained on a large data set of synthetic measurements, is applied to perform aerosol retrievals from real RSP data, and the neural network retrievals are subsequently used as a first guess for the Phillips–Tikhonov retrieval. The resulting algorithm appears capable of accurately retrieving aerosol optical thickness, fine-mode effective radius and aerosol layer height from RSP data. Among the advantages of using a neural network as initial guess for an iterative algorithm are a decrease in processing time and an increase in the number of converging retrievals.