Ammonia loss results in significant resource waste and environmental pollution. In this study, we proposed and explored the way of using air plasmas to capture NH3 to form NH4NO3 for N recycling under different reaction modes, discharge powers, and gas flow rates. The reaction mechanisms under different modes were also revealed. A needle-needle discharge driven by AC power was used and ammonia gas was utilized to simulate the volatilized ammonia. Notably, white particles were observed during Mode 1 and Mode 2 (these particles gradually disappeared over time in Mode 2), while no particles or significant NOx were detected in Mode 3 throughout the process. The quantitative NH4NO3 yield was significantly influenced by discharge power and NH3 flow rate, reaching its highest value in Mode 1 at 24 W and 20 sccm in this investigation. Directly mixing the air discharge products with NH3 in Mode 1 under the threshold decomposition temperature of NH4NO3 leads to the stable formation of NH4NO3. Discharging in the NH3/air mixture will inhibit the generation of NOx and further restrain the NH4NO3 formation in Mode 2 and 3. Additionally, the temperature rises during discharge and also decomposes NH4NO3, resulting in unstable NH4NO3 formation in Mode 2.