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We present the first observational study on the potential of band-differenced angular signatures for cloud detection. A band-differenced angular signature is the reflectance difference between the blue and near-infrared channels examined as a function of view angle, and it is observed in this study from the Multi-angle Imaging SpectroRadiometer (MISR). The observed band-differenced angular signatures over a variety of scene types qualitatively compare well with previously published theoretical predictions. Examples of cloud detection in polar and desert regions using band-differenced angular signatures from MISR are shown to highlight its contribution to cloud detection in areas where traditional spectral techniques tend to perform poorly.