Widespread mobilization of nitrogen into the atmosphere from industry, agriculture, and biomass burning and its subsequent deposition have the potential to alleviate nitrogen limitation of productivity in terrestrial ecosystems, and may contribute to enhanced terrestrial carbon uptake. To evaluate the importance of the spatial distribution of nitrogen deposition for carbon uptake and to better quantify its magnitude and uncertainty NOy-N deposition fields from five different three-dimensional chemical models, GCTM, GRANTOUR, IMAGES, MOGUNTIA, and ECHAM were used to drive NDEP, a perturbation model of terrestrial carbon uptake. Differences in atmospheric sources of NOx-N, transport, resolution, and representation of chemistry, contribute to the distinct spatial patterns of nitrogen deposition on the global land surface; these differences lead to distinct patterns of carbon uptake that vary between 0.7 and 1.3 Gt C yr−1 globally. Less than 10% of the nitrogen was deposited on forests which were most able to respond with increased carbon storage because of the wide C:N ratio of wood as well as its long lifetime. Addition of NHx-N to NOy-N deposition, increased global terrestrial carbon storage to between 1.5 and 2.0 Gt C yr−1, while the “missing terrestrial sink” is quite similar in magnitude. Thus global air pollution appears to be an important influence on the global carbon cycle. If N fertilization of the terrestrial biosphere accounts for the “missing” C sink or a substantial portion of it, we would expect significant reductions in its magnitude over the next century as terrestrial ecosystems become N saturated and O3 pollution expands.