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Imaging spectroscopy is a powerful technique for monitoring the biochemical constituents of vegetation and is critical for understanding the fluxes of carbon and water between the land surface and the atmosphere. However, spectral observations are subject to the sun-observer geometry and canopy structure which impose confounding effects on spectral estimates of leaf pigments. For instance, the sun-observer geometry influences the spectral brightness measured by the sensor. Likewise, when considering pigment distribution at the stand level scale, the pigment content observed from single view angles may not necessarily be representative of stand-level conditions as some constituents vary as a function of the degree of leaf illumination and are therefore not isotropic. As an alternative to mono-angle observations, multi-angular remote sensing can describe the anisotropy of surface reflectance and yield accurate information on canopy structure. These observations can also be used to describe the bi-directional reflectance distribution which then allows the modeling of reflectance independently of the observation geometry. In this paper, we demonstrate a method for estimating pigment contents of chlorophyll and carotenoids continuously over a year from tower-based, multi-angular spectro-radiometer observations. Estimates of chlorophyll and carotenoid content were derived at two flux-tower sites in western Canada. Pigment contents derived from inversion of a CR model (PROSAIL) compared well to those estimated using a semi-analytical approach (r2 = 0.90 and r2 = 0.69, P < 0.05 for both sites, respectively). Analysis of the seasonal dynamics indicated that net ecosystem productivity was strongly related to total canopy chlorophyll content at the deciduous site (r2 = 0.70, P < 0.001), but not at the coniferous site. Similarly, spectral estimates of photosynthetic light-use efficiency showed strong seasonal patterns in the deciduous stand, but not in conifers. We conclude that multi-angular, spectral observations can play a key role in explaining seasonal dynamics of fluxes of carbon and water and provide a valuable addition to flux-tower-based networks.