Leaf nitrogen and leaf surface area influence the exchange of gases between terrestrial ecosystems and the atmosphere, and they play a significant role in the global cycles of carbon, nitrogen and water. Remote sensing data from satellites can be used to estimate leaf area index (LAI), leaf chlorophyll (CHLl) and leaf nitrogen density (Nl). However, methods are often developed using plot scale data and not verified over extended regions that represent a variety of soil spectral properties and canopy structures. In this paper, field measurements and high spatial resolution (10–20 m) remote sensing images acquired from the HRG and HRVIR sensors aboard the SPOT satellites were used to assess the predictability of LAI, CHLl and Nl. Five spectral vegetation indices (SVIs) were used (the Normalized Difference Vegetation index, the Simple Ratio, the Enhanced Vegetation Index-2, the Green Normalized Difference Vegetation Index, and the green Chlorophyll Index) together with the image-based inverse canopy radiative transfer modelling system, REGFLEC (REGularized canopy reFLECtance). While the SVIs require field data for empirical model building, REGFLEC can be applied without calibration. Field data measured in 93 fields within crop- and grasslands of five European landscapes showed strong vertical CHLl gradient profiles in 20% of fields. This affected the predictability of SVIs and REGFLEC. However, selecting only homogeneous canopies with uniform CHLl distributions as reference data for statistical evaluation, significant (p < 0.05) predictions were achieved for all landscapes, by all methods. The best performance was achieved by REGFLEC for LAI (r2=0.7; rmse = 0.73), canopy chlorophyll content (r2=0.51; rmse = 439 mg m−2) and canopy nitrogen content (r2 = 0.53; rmse = 2.21 g m−2). Predictabilities of SVIs and REGFLEC simulations generally improved when constrained to single land use categories (wheat, maize, barley, grass) across the European landscapes, reflecting sensitivity to canopy structures. Predictability further improved when constrained to local (10 × 10 km2) landscapes, thereby reflecting sensitivity to local environmental conditions. All methods showed different predictabilities for land use categories and landscapes. Combining the best methods, LAI, canopy chlorophyll content (CHLc) and canopy nitrogen content (CHLc) for the five landscapes could be predicted with improved accuracy (LAI rmse = 0.59; CHLc rmse = 346 g m−2; Ncrmse = 1.49 g m−2). Remote sensing-based results showed that the vegetation nitrogen pools of the five agricultural landscapes varied from 0.6 to 4.0 t km−2. Differences in nitrogen pools were attributed to seasonal variations, extents of agricultural area, species variations, and spatial variations in nutrient availability. Information on Nl and total Nc pools within the landscapes is important for the spatial evaluation of nitrogen and carbon cycling processes. The upcoming Sentinel-2 satellite mission will provide new multiple narrow-band data opportunities at high spatio-temporal resolution which are expected to further improve remote sensing predictabilities of LAI, CHLl and Nl.