Excessive ammonia (NH3) emitted from nitrogen (N) fertilizer applications in global croplands plays an important role in atmospheric aerosol production, resulting in visibility reduction and regional haze. However, large uncertainty exists in the estimates of NH3 emissions from global and regional croplands, which utilize different data and methods. In this study, we have coupled a process‐based Dynamic Land Ecosystem Model (DLEM) with the bidirectional NH3 exchange module in the Community Multiscale Air‐Quality (CMAQ) model (DLEM‐Bi‐NH3) to quantify NH3 emissions at the global and regional scale, and crop‐specific NH3 emissions globally at a spatial resolution of 0.5° × 0.5° during 1961–2010. Results indicate that global NH3 emissions from N fertilizer use have increased from 1.9 ± 0.03 to 16.7 ± 0.5 Tg N/year between 1961 and 2010. The annual increase of NH3 emissions shows large spatial variations across the global land surface. Southern Asia, including China and India, has accounted for more than 50% of total global NH3 emissions since the 1980s, followed by North America and Europe. Rice cultivation has been the largest contributor to total global NH3 emissions since the 1990s, followed by corn and wheat. In addition, results show that empirical methods without considering environmental factors (constant emission factor in the IPCC Tier 1 guideline) could underestimate NH3 emissions in context of climate change, with the highest difference (i.e., 6.9 Tg N/year) occurring in 2010. This study provides a robust estimate on global and regional NH3 emissions over the past 50 years, which offers a reference for assessing air quality consequences of future nitrogen enrichment as well as nitrogen use efficiency improvement. Based on the process‐based DLEM‐Bi‐NH3 module, global NH3 emissions from N fertilizer use have increased by 14.8 Tg N/year during the period 1961–2010. At the regional scale, southern Asia, including China and India, has accounted for more than 50% of total global NH3 emissions since the 1980s. Rice cultivation has been the largest contributor to total global NH3 emissions since the 1990s, followed by corn and wheat. In addition, results show that empirical methods without considering environmental factors (constant emission factor in the IPCC Tier 1 guideline) could underestimate NH3 emissions in the context of climate change, with the highest difference (i.e., 6.9 Tg N/year) occurring in 2010.