This bottom-up modeling study, supported by new population census 2011 data, simulates ozone (O3) and fine particulate matter (PM2.5) exposure on local to regional scales. It quantifies, present-day premature mortalities associated with the exposure to near-surface PM2.5 and O3 concentrations in India using a regional chemistry model. We estimate that PM2.5 exposure leads to about 570,000 (CI95: 320,000–730,000) premature mortalities in 2011. On a national scale, our estimate of mortality by chronic obstructive pulmonary disease (COPD) due to O3 exposure is about 12,000 people.