Foliar nitrogen has been shown to be positively correlated with midsummer canopy albedo and canopy near infrared (NIR) reflectance over a broad range of plant functional types (e.g., forests, grasslands, and agricultural lands). To date, the mechanism(s) driving the nitrogen–albedo relationship have not been established, and it is unknown whether factors affecting nitrogen availability will also influence albedo. To address these questions, we examined variation in foliar nitrogen in relation to leaf spectral properties, leaf mass per unit area, and leaf water content for three deciduous species subjected to either nitrogen (Harvard Forest, MA, and Oak Ridge, TN) or CO(2) fertilization (Oak Ridge, TN). At Oak Ridge, we also obtained canopy reflectance data from the airborne visible/infrared imaging spectrometer (AVIRIS) to examine whether canopy-level spectral responses were consistent with leaf-level results. At the leaf level, results showed no differences in reflectance or transmittance between CO(2) or nitrogen treatments, despite significant changes in foliar nitrogen. Contrary to our expectations, there was a significant, but negative, relationship between foliar nitrogen and leaf albedo, a relationship that held for both full spectrum leaf albedo as well as leaf albedo in the NIR region alone. In contrast, remote sensing data indicated an increase in canopy NIR reflectance with nitrogen fertilization. Collectively, these results suggest that altered nitrogen availability can affect canopy albedo, albeit by mechanisms that involve canopy-level processes rather than changes in leaf-level reflectance.