The present study reports spatio-temporal distribution pattern of major gaseous (NH3 and NO2) and particulate water soluble total nitrogen (pWSTN) in the ambient air to explore the seasonal variation, major interactions and dominating sources. Considering the major hotspot of atmospheric reactive nitrogen (N) emission, three sites in Indo-Gangetic plain (IGP) were selected based on different local source parameters. Results have shown that gas phase reactive N contribute up to 90% of total analyzed reactive N, where NH3 imparted highest at all the three sites. Prayagraj, a fast growing urban site, has shown highest concentrations of NH3 (72.0 μg m−3), followed by Madhupur rural site (57.7 μg m−3) and Delhi, an urban megacity site (35.8 μg m−3). As compared to previous studies conducted at different sites of IGP, NH3 concentrations were reported to be the highest at the former two sites. However, unlike NH3, NO2 levels were recorded lower at Madhupur (3.1 μg m−3) and Prayagraj (9.4 μg m−3) sites as compared to Delhi (13.4 μg m−3). Similarly, pWSTN concentrations were in the order of Madhupur (6.6 μg m−3) < Prayagraj (10.0 μg m−3) < Delhi (10.1 μg m−3). A strong correlation of NO2 with pWSTN at urban sites has shown the crucial role of NO2 in the formation of nitrogenous aerosols. Significant spatial variation can be attributed to varying local emission sources ranging from microbial emission from improper sewage treatment and open waste dumping at Prayagraj, agricultural activities at Madhupur and vehicular exhausts at Delhi site.