Aerosol-induced perturbations in cloud systems and rainfall are very uncertain. This study provides observational evidence of a robust positive association between aerosol–cloud–rainfall properties over the Indian summer monsoon region. Observed and modeled aerosol–cloud microphysical changes illustrate that cloud invigoration under a high AOD scenario can explain most of the aerosol-associated changes in cloud fraction, cloud top pressure, and surface rainfall over this region.