Although lunar studies suggest that large asteroid impact rates in the inner solar system declined to their present low levels at 3.8–3.7 Ga, recent studies in greenstone belts indicate that asteroids 20 km to 70+ km in diameter were still striking the Earth as late as 3.2 Ga at rates significantly greater than the values estimated from lunar studies. We here present geologic evidence that two of these terrestrial impacts, at 3.29 Ga and 3.23 Ga, caused heating of Earth’s atmosphere, ocean-surface boiling, and evaporation of tens of meters to perhaps 100 m of seawater. Rapid ocean evaporation resulted in abrupt sea-level drops, erosion of the exposed sea floor, and precipitation of distinctive layers of laminated silica representing marine siliceous sinter. Such events would have severely affected microbial communities, especially among shallow-water and photosynthetic organisms. These large impacts profoundly affected Archean crustal development, surface environment, and biological evolution until 3.2 Ga, or even later.