More than four decades of research provide unequivocal evidence that sulfur, nitrogen, and mercury pollution have altered, and will continue to alter, our nation's lands and waters. The emission and deposition of air pollutants harm native plants and animals, degrade water quality, affect forest productivity, and are damaging to human health. Many air quality policies limit emissions at the source but these control measures do not always consider ecosystem impacts. Air pollution thresholds at which ecological effects are observed, such as critical loads, are effective tools for assessing the impacts of air pollution on essential ecosystem services and for informing public policy. U.S. ecosystems can be more effectively protected and restored by using a combination of emissions-based approaches and science-based thresholds of ecosystem damage.