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The recent availability of quasi-simultaneous multispectral and multidirectional measurements from space, as provided by the Multi-angle Imaging SpectroRadiometer (MISR) on board the Terra platform, offers new and unique opportunities to document the anisotropy of land surfaces at critical solar wavelengths. This paper presents simple physical principles supporting the interpretation of the anisotropy of spectral radiances exiting terrestrial surfaces in terms of a signature of surface heterogeneity. The shape of the anisotropy function is represented with two model parameter values which may be mapped and interpreted in their own right. The value of one of these parameters also permits identifying geophysical conditions where the surface heterogeneity becomes significant and where three-dimensional (3D) radiation transfer effects have to be explicitly accounted for. This paper documents these findings on the basis of results from a number of 3D radiation transfer model simulations. The latter are used to perform an extensive sensitivity study which includes issues related to the scale of investigation. A preliminary validation of these results, conducted with a dataset collected by the AirMISR instrument over the Konza prairie, is also discussed.