Despite the proliferation of control technologies, air pollution remains a major concern across the United States, suggesting the need for a paradigm shift in methods for mitigating emissions. Based on data about annual emissions in U.S. counties and current land cover, we show that existing forest, grassland, and shrubland vegetation take up a significant portion of current U.S. emissions. Restoring land cover, where possible, to county-level average canopy cover can further remove pollution of SO2, PM10, PM2.5, and NO2 by an average of 27% through interception of particulate matter and absorption of gaseous pollutants. We find such nature-based solutions to be cheaper than technology for several National Emission Inventory sectors. Our results with and without monetary valuation of ecological cobenefits identify sectors and counties that are most economically attractive for nature-based solutions as compared to the use of pollution control technologies. We also estimate the sizes of urban and rural populations that would benefit from this novel ecosystem-based approach. This suggests that even though vegetation cannot fully negate the impact of emissions at all times, policies encouraging ecosystems as control measures in addition to technological solutions may promote large investments in ecological restoration and provide several societal benefits.