Exposure to ambient fine particulate matter (PM2.5) is a leading contributor to diseases in India. Previous studies analysing emission source attributions were restricted by coarse model resolution and limited PM2.5 observations. We use a regional model informed by new observations to make the first high-resolution study of the sector-specific disease burden from ambient PM2.5 exposure in India. Observed annual mean PM2.5 concentrations exceed 100 μg m-3 and are well simulated by the model. We calculate that the emissions from residential energy use dominate (52%) population-weighted annual mean PM2.5 concentrations, and are attributed to 511,000 (95UI: 340,000-697,000) premature mortalities annually. However, removing residential energy use emissions would avert only 256,000 (95UI: 162,000-340,000), due to the non-linear exposure-response relationship causing health effects to saturate at high PM2.5 concentrations. Consequently, large reductions in emissions will be required to reduce the health burden from ambient PM2.5 exposure in India.