Extreme weather events have become more frequent and are likely linked to increases in greenhouse gases and aerosols, which alter the Earth's radiative balance and cloud processes. On 8–9 July 2013, a catastrophic flood devastated the mountainous area to the northwest of the Sichuan Basin. Atmospheric simulations at a convection-permitting scale with aerosols and chemistry included show that heavy air pollution trapped in the basin significantly enhances the rainfall intensity over the mountainous areas through “aerosol-enhanced conditional instability.” That is, aerosols suppress convection by absorbing solar radiation and increasing atmospheric stability in the basin during daytime. This allows excess moist air to be transported to the mountainous areas and orographically lifted, generating strong convection and extremely heavy precipitation at night. We show that reducing pollution in the Sichuan Basin can effectively mitigate floods. It is suggested that coupling aerosol with meteorology can be crucial to improve weather forecast in polluted regions.