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In this paper, the potential of Compact High-Resolution Imaging Spectrometer (CHRIS)/Project for On-Board Autonomy data for impervious surface mapping is tested in a mixed urban/suburban/rural environment including part of the city of Leuven (Belgium) using multiple endmember unmixing. Various unmixing scenarios are compared, using different threshold values for the RMSE criterion applied to select the proper model for unmixing each pixel. Validation based on 25-cm aerial photography shows that the use of threshold values that favor the application of models with a small number of endmembers performs better compared to scenarios that make use of models with more endmembers. Detailed analysis of model selection for pixels with different land-cover composition indicates that the error in fraction estimation is partly related to spectral confusion between impervious surface types and bare soil, leading to the selection of inappropriate models for the unmixing. In spite of the spectral similarity of soil and impervious surface endmembers, average fractional error for impervious surfaces, vegetation, and bare soil is around 15%, which demonstrates the potential of CHRIS data for mapping the major physical components of the urban/suburban environment at the subpixel scale.