Hydroxyl radical (·OH) plays a crucial role in atmospheric chemistry, regulating the oxidative potential and aerosol composition. This study reveals an unprecedented source of ·OH in the atmosphere: mineral dust-bearing microdroplet aerosols. We demonstrate that Kaolin clay particles in microdroplet aerosols trigger rapid ·OH production upon solar irradiation, with rates reaching an order of at least 10-3 M s-1. This production rate is several orders of magnitude higher than that of the bulk phase (2.4 × 10-11 M s-1) and previously known pathways. On this basis, the surface-based interfacial ·OH production rate is estimated to be 8.9 × 10-5 mol m-2 s-1 at the air-water-solid interface of 1 μm sized aerosol particles. The enhanced ·OH formation is attributed to the unique features of air-water-solid interfaces, where the lifespan of photoinduced holes was significantly increased due to the presence of strong electric fields at the air-water interface. We further investigated the impacts of various environmental factors and aerosol properties on ·OH production, including light intensity, relative humidity, particle size, and pH. Our findings provide new insights into atmospheric photochemical processes mediated by mineral dust-bearing microdroplet aerosols, which are important contributors to ·OH source in the atmosphere. This work advances our understanding of atmospheric interfacial chemistry and its profound and lasting implications for air quality and climate.