Nitrogen (N) pollution is shaped by multiple processes, the combined effects of which remain uncertain, particularly in the tropics. We use a global land biosphere model to analyze historical terrestrial-freshwater N budgets, considering the effects of anthropogenic N inputs, atmospheric CO2, land use, and climate. We estimate that globally, land currently sequesters 11 (10–13)% of annual N inputs. Some river basins, however, sequester >50% of their N inputs, buffering coastal waters against eutrophication and society against greenhouse gas-induced warming. Other basins, releasing >25% more than they receive, are mostly located in the tropics, where recent deforestation, agricultural intensification, and/or exports of land N storage can create large N pollution sources. The tropics produce 56 ± 6% of global land N pollution despite covering only 34% of global land area and receiving far lower amounts of fertilizers than the extratropics. Tropical land use should thus be thoroughly considered in managing global N pollution.