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Viewing and illumination geometry has a strong influence on optical measurements of natural surfaces due to their anisotropic reflectance properties. Typically, cameras on-board unmanned aerial vehicles (UAVs) are affected by this because of their relatively large field of view (FOV) and thus large range of viewing angles. In this study, we investigated the magnitude of reflectance anisotropy effects in the 500–900 nm range, captured by a frame camera mounted on a UAV during a standard mapping flight. After orthorectification and georeferencing of the images collected by the camera, we calculated the viewing geometry of all observations of each georeferenced ground pixel, forming a dataset with multi-angular observations. We performed UAV flights on two days during the summer of 2016 over an experimental potato field where different zones in the field received different nitrogen fertilization treatments. These fertilization levels caused variation in potato plant growth and thereby differences in structural properties such as leaf area index (LAI) and canopy cover. We fitted the Rahman–Pinty–Verstraete (RPV) model through the multi-angular observations of each ground pixel to quantify, interpret, and visualize the anisotropy patterns in our study area. The Θ parameter of the RPV model, which controls the proportion of forward and backward scattering, showed strong correlation with canopy cover, where in general an increase in canopy cover resulted in a reduction of backward scattering intensity, indicating that reflectance anisotropy contains information on canopy structure. In this paper, we demonstrated that anisotropy data can be extracted from measurements using a frame camera, collected during a typical UAV mapping flight. Future research will focus on how to use the anisotropy signal as a source of information for estimation of physical vegetation properties.