Daily simulations of tropospheric carbon monoxide (CO) and ozone (O3) have been made using MOZART-4 (Model for OZone And Related chemical Tracers version 4) during 2007–08. The model simulated CO and O3 are evaluated against MOZAIC (Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft) airborne observations over Hyderabad and IASI (Infrared Atmospheric Sounding Interferometer) retrievals over five most populous cities of India i.e. Mumbai, Delhi, Bangalore, Hyderabad, and Ahmedabad. The MOZAIC tropospheric column showed winter maxima and summer minima for CO whereas spring maxima and summer minima for O3. These seasonal features are reproduced well by model over Hyderabad. Model lower and middle tropospheric CO (O3) columns are positively biased by about 14 (8) ppbv as compared to MOZAIC observations. Model underestimated (overestimated) IASI CO columns during pre-monsoon (post-monsoon) while it overestimated IASI O3 columns throughout the year. Model simulated column of CO and O3 are positively biased by 4–13% and 23–33% respectively as compared to the IASI retrievals over five most populous cities. Tagged and sensitivity simulations of MOZART-4 have been used to quantify the contribution of different sources to the tropospheric CO and O3 distribution over the Indian landmass region. At surface, anthropogenic contribution varies from 55% to 81% during different seasons with an annual average contribution of 67%. This contribution decreases with increasing altitude up to 35% at 300 hPa. The contribution of photochemically produced CO is found to be 9–33% at surface. Unlike ANT-CO, the photochemically produced CO increases with altitude as it reaches up to 48% at 300 hPa. Surface BB-CO contributes upto 30% over parts of North East India during pre-monsoon season. Contribution of NAT-CO is found to be negligible (Approximately 6%) near surface as well as at the higher altitudes. Sensitivity simulations are used to decompose the total ozone (TO) into contributions from enhancement of ozone from Indian anthropogenic emissions, referred as Indian pollution ozone (IPO) and from the total background ozone (TBO). Annual total ozone is found to be 30 to 70 ppbv at surface and 77 to 85 ppbv at 300 hPa over the Indian landmass region. IPO and TBO contribute annually 58% and 42% at surface while 45% and 55% at 300 hPa respectively. The IPO contributes strongly at surface, with maximum (68%) impact during pre-monsoon season.