The air quality of national capital region (NCR) of Delhi, India is becoming more severe day by day because of the anthropogenic activities. To get a better understanding of the ambient air quality of NCR-Delhi, the study of carbonaceous species in particulate matter (PM) is essential. PM10 samples were collected periodically from the three main urban sites (Faridabad; IGDTUW-Delhi; and CSIR-NPL Delhi,) of NCR-Delhi in the year 2015 to explore the possible sources of carbonaceous species [organic carbon (OC), elemental carbon (EC), and water-soluble organic carbon (WSOC)] in PM10. The annual average concentrations of PM10, OC, EC, and WSOC were estimated as 195 ± 121, 23.6 ± 14.4, 5.2 ± 4.0, and 15.5 ± 7.7 µg m−3, respectively, at Faridabad, whereas average concentrations of PM10, OC, EC, and WSOC were 274 ± 141, 30.8 ± 19.3, 9.4 ± 5.2, and 21.3 ± 14.3 µg m−3, respectively, at IGDTUW, Kashmiri Gate. Concentrations of PM10, OC, EC and WSOC were estimated as 209 ± 81, 26.0 ± 12.8, 7.9 ± 5.6 and 9.7 ± 5.9 µg m−3 at CSIR-NPL. During the study, a significant positive linear trend between OC vs. EC and OC vs. WSOC have been observed for these three sites as (R2 = 0.64 and R2 = 0.76 at Faridabad; R2 = 0.66 and R2 = 0.87 at IGDTUW-Delhi; and R2 = 0.79 and R2= 0.55 at CSIR-NPL), which indicates the common sources (vehicular emission and/or biomass burning) of carbonaceous aerosols over NCR-Delhi. All these carbonaceous species of PM10 shows seasonal variation with maxima during winter as well as post-monsoon and minima during monsoon seasons. 5 days backward trajectories of the air masses were calculated which shows the origination of pollutants from local sources along with long-range transport. Furthermore, the secondary and primary organic carbon (i.e., SOC and POC) in PM10 were also computed and reported.