Agra and Kanpur are heavily polluted Indian cities and are the fourth and second largest cities in Uttar Pradesh State, respectively. PM2.5 was collected from December 2011 to May 2012 in Agra and from December 2011 to October 2012 in Kanpur every 6th day. The samples were chemically analyzed to determine organic carbon (OC), water soluble organic carbon (WSOC), elemental carbon (EC), secondary inorganic ions, and particle–phase organic compounds. A chemical mass balance (CMB) receptor model using organic tracers was used to estimate source contributions to PM2.5. Concentrations of carbonaceous aerosols were on average 23±16 mg/m3 in Agra and 33±21 mg/m3 in Kanpur during the winter and summer periods, and had a strong seasonal trend with highest levels in winter (December–February) and then decreasing to summer (March–May). Five primary sources were identified. In Agra, biomass burning was the major source of OC in the winter months with decreasing relative and absolute concentrations in summer. In Kanpur, biomass burning was also the most important primary source of OC, but was about half the concentration found in Agra. Mobile source contributions to OC were on average 25±9% and 25±22% in Agra and Kanpur, respectively, with similar absolute concentrations of 2.5±1.9 mg/m3 in most months. Secondary organic aerosol (SOA) was estimated from non–biomass burning WSOC and the unapportioned OC, with each method indicating SOA as a major source of OC in the winter in both cities, apportioning 25% of OC in Agra and 65% in Kanpur. SOA in Kanpur in December was four times higher than in Agra. Overall, results suggest differences in aerosol chemical composition and sources at these two sites across the Indo–Gangetic plain with biomass burning making up a larger fraction of the particulate OC in Agra, and SOA being a more important contributor to OC mass in Kanpur.