In this study, we categorized detailed mass-based emission factors (EFs) by age, calculated new estimates of fuel use, and developed spatially resolved emission inventories of constituents (PM2.5, black carbon [BC], and organic carbon [OC]) in the fine aerosol generated by the on-road transport sector in India. On a national level, this sector released an estimated 355 (104–607) Gg y–1, 137 (47–227) Gg y–1, and 106 (34–178) Gg y–1 of PM2.5, BC, and OC, respectively, for the base year 2013, contributing nearly 7%, 17%, and 6% of the total emissions for each constituent. Although super-emitter vehicles comprised only 24% of the total traffic volume, they were responsible for 67% and 47% of the national PM2.5 and BC emissions, respectively, which indicates that eliminating these vehicles may rapidly reduce emissions from the on-road transport sector in India. To predict the direct radiative forcing (DRF) from BC emissions in this sector, we then input emission estimates for the carbonaceous aerosols into the Community Atmosphere Model (CAM5) global climate model and found a positive DRF of up to 6 W m–2 at the top of the atmosphere (TOA) and a negative DRF of up to 10 W m–2 at the surface, suggesting that as much as 16 W m–2 of energy remains trapped within the atmosphere. With the rapid economic growth and continued urbanization, the transport sector in India is likely to further expand in the future and hence requires immediate attention in order to reduce the BC burden and improve air quality in the nation.