National Capital Territory of Delhi and its satellite cities suffer from poor air quality during the post-monsoon months of October–November. In this study, a novel attempt is made to estimate the contribution of different emission sources (industrial, residential, power generation, transportation, biomass burning, photochemical production, lateral transport, etc.) towards the criteria air pollutant carbon monoxide (CO) concentration over North India. Multiple simulations of the WRF-Chem model with a tagged tracer approach with different inputs (6 anthropogenic emission inventories and 3 biomass burning emission inventories) were used. The model performance was evaluated against the MOPITT retrieved CO surface concentration. Analysis of model simulated CO over North India suggests that anthropogenic emissions contribute around 32–49% to surface CO concentration while crop residue burning contributes 27–44% of which 80% originates from Punjab. For Delhi, the contribution from anthropogenic sources is dominant (53–77%) of which 10–28% is from the domestic sector and 14–55% is from the transport sector. Agricultural waste burning contributes about 15–30% to Delhi's surface CO concentration (of which 75% originates from Punjab). Crop residue burning emission is a chief source of CO over Punjab with a contribution of about 56–76%. The results suggest that industrial, transport, and domestic sector activities are more responsible for increased CO levels over New Delhi and surrounding regions than crop residue burning over Punjab. Furthermore, critical meteorological parameters like 10 m wind speed, boundary layer height, 2 m temperature, total precipitation, and relative humidity were evaluated against CO concentration to understand their impact on CO distribution. Results conclude that deteriorating air quality over the North Indian region is caused by a combination of prevailing meteorological factors (such as slow winds, shallow mixing layer, and cold temperatures) and man-made emissions.