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• Soil carbon sequestration was significantly increased by long-term N addition. • NECB and NGWP were significantly reduced by long-term N addition. • The offset effect of N 2 O emissions to ecosystem C uptake was decreased by LN addition. Grassland systems are important terrestrial carbon sinks and have great potential for carbon (C) sequestration. Increased atmospheric nitrogen (N) deposition has profoundly affected C balance and greenhouse gas emissions in grassland systems. However, the effects of long-term nitrogen (LN) deposition on net ecosystem carbon budget (NECB) and net global warming potential (NGWP) in grassland systems are still not clearly understood. A field experiment was conducted to test the effect of LN addition (0, 30, 60, 120 and 240 kg N ha−1 yr−1) on NECB and NGWP in a temperate grassland area in Inner Mongolia, China. LN addition significantly increased soil organic carbon density (SOCD) and C sequestration in surface soil (0–30 cm) with the increase of N addition rate from 2005 to 2018. In contrast, a decrease in ecosystem respiration (R e) was observed, except at low LN concentration (30 kg N ha−1 yr−1). Annual N 2 O flux was significantly increased, and the CH 4 sink was significantly decreased by LN addition. NECB and NGWP were relatively weak in this temperate grassland, ranging from −627.29 ± 198.81 and −232.87 ± 23.11 kg CO 2 ha−1yr−1, respectively, and significantly decreased with increasing LN application. The offset effect of N 2 O emission to ecosystem C uptake decreased significantly with increased LN addition, and was stable at high LN addition. This was related to the increase in soil C sequestration due to plant C uptake. These results indicate that LN addition significantly decreased the NECB and NGWP of this grassland. Increased long-term N deposition significantly enhanced soil C sequestration, which has important implications for mitigating climate warming. [ABSTRACT FROM AUTHOR]