Interactions between the terrestrial nitrogen (N) and carbon (C) cycles shape the response of ecosystems to global change. However, the global distribution of nitrogen availability and its importance in global biogeochemistry and biogeochemical interactions with the climate system remain uncertain. Based on projections of a terrestrial biosphere model scaling ecological understanding of nitrogen–carbon cycle interactions to global scales, anthropogenic nitrogen additions since 1860 are estimated to have enriched the terrestrial biosphere by 1.3 Pg N, supporting the sequestration of 11.2 Pg C. Over the same time period, CO2 fertilization has increased terrestrial carbon storage by 134.0 Pg C, increasing the terrestrial nitrogen stock by 1.2 Pg N. In 2001–2010, terrestrial ecosystems sequestered an estimated total of 27 Tg N yr−1 (1.9 Pg C yr−1), of which 10 Tg N yr−1 (0.2 Pg C yr−1) are due to anthropogenic nitrogen deposition. Nitrogen availability already limits terrestrial carbon sequestration in the boreal and temperate zone, and will constrain future carbon sequestration in response to CO2 fertilization (regionally by up to 70% compared with an estimate without considering nitrogen–carbon interactions). This reduced terrestrial carbon uptake will probably dominate the role of the terrestrial nitrogen cycle in the climate system, as it accelerates the accumulation of anthropogenic CO2 in the atmosphere. However, increases of N2O emissions owing to anthropogenic nitrogen and climate change (at a rate of approx. 0.5 Tg N yr−1 per 1°C degree climate warming) will add an important long-term climate forcing.