Identifying the sources of reactive nitrogen (N) and quantifying their contributions to groundwater nitrate concentrations are critical to understanding the dynamics of groundwater nitrate contamination. Here we assessed groundwater nitrate contamination in China using literature analysis and N balance calculation in coupled human and natural systems. The source appointment via N balance was well validated by field data via literature analysis. Nitrate was detected in 96% of groundwater samples based on a common detection threshold of 0.2 mg N L-1, and 28% of groundwater samples exceeded WHO’s maximum contaminant level (10 mg N L-1). Groundwater nitrate concentrations were the highest beneath industrial land (median: 34.6 mg N L-1), followed by urban land (10.2 mg N L-1), cropland (4.8 mg N L-1), and rural human settlement (4.0 mg N L-1), with the lowest found beneath natural land (0.8 mg N L-1). During the period 1980-2008, total reactive N leakage to groundwater increased about 1.5 times, from 2.0 to 5.0 Tg N yr-1, in China. Despite that the contribution of cropland to the total amount of reactive N leakage to groundwater was reduced from 50 to 40% during the past three decades, cropland still was the single largest source, while the contribution from landfill rapidly increased from 10 to 34%. High reactive N leakage mainly occurred in relatively developed agricultural or urbanized regions with a large population. The amount of reactive N leakage to groundwater was mainly driven by anthropogenic factors (population, gross domestic product, urbanization rate and land use type). We constructed a high resolution map of reactive N source appointment and this could be the basis for future modeling of groundwater nitrate dynamics and for policy development on mitigation of groundwater contamination.