Nitrogen (N) availability plays a key role in terrestrial biosphere dynamics. To understand and quantify the role of terrestrial N in the Earth system, we developed an advanced terrestrial biogeochemical model O-CN that mechanistically couples terrestrial energy, water, carbon, and nitrogen fluxes in terrestrial ecosystems. We evaluate this new model against observations from intensive forest monitoring plots at temperate and boreal locations in Europe. O-CN simulates realistic foliage N concentrations and N cycling rates and reproduces observed diurnal and seasonal cycles of C fluxes as well as observed gradients in vegetation productivity with N availability for the forest sites studied. A sensitivity test reveals that these results are reasonably robust against uncertainties in model parameter estimates. Using this model we quantify the likely contribution of anthropogenic N deposition to present ecosystem C sequestration as 36 (range: 2–79) g C g−1 N in agreement with ecosystem manipulation studies.