The Yangtze River basin is one of the world's hotspots for nitrogen (N) deposition and likely plays an important role in China's riverine N output. Here we constructed a basin-scale total dissolved inorganic N (DIN) deposition (bulk plus dry) pattern based on published data at 100 observational sites between 2000 and 2014, and assessed the relative contributions of different reactive N (N) emission sectors to total DIN deposition using the GEOS-Chem model. Our results show a significant spatial variation in total DIN deposition across the Yangtze River basin (33.2 kg N ha yr on average), with the highest fluxes occurring mainly in the central basin (e.g., Sichuan, Hubei and Hunan provinces, and Chongqing municipality). This indicates that controlling N deposition should build on mitigation strategies according to local conditions, namely, implementation of stricter control of N emissions in N deposition hotspots but moderate control in the areas with low N deposition levels. Total DIN deposition in approximately 82% of the basin area exceeded the critical load of N deposition for semi-natural ecosystems along the basin. On the basin scale, the dominant source of DIN deposition is fertilizer use (40%) relative to livestock (11%), industry (13%), power plant (9%), transportation (9%), and others (18%, which is the sum of contributions from human waste, residential activities, soil, lighting and biomass burning), suggesting that reducing NH emissions from improper fertilizer (including chemical and organic fertilizer) application should be a priority in curbing N deposition. This, together with distinct spatial variations in emission sector contributions to total DIN deposition also suggest that, in addition to fertilizer, major emission sectors in different regions of the basin should be considered when developing synergistic control measures.