Rising atmospheric carbon dioxide (CO2) levels, from fossil fuel combustion and deforestation, along with agriculture and land-use practices are causing wholesale increases in seawater CO2 and inorganic carbon levels; reductions in pH; and alterations in acid-base chemistry of estuarine, coastal, and surface open-ocean waters. On the basis of laboratory experiments and field studies of naturally elevated CO2 marine environments, widespread biological impacts of human-driven ocean acidification have been posited, ranging from changes in organism physiology and population dynamics to altered communities and ecosystems. Acidification, in conjunction with other climate change–related environmental stresses, particularly under future climate change and further elevated atmospheric CO2 levels, potentially puts at risk many of the valuable ecosystem services that the ocean provides to society, such as fisheries, aquaculture, and shoreline protection. This review emphasizes both current scientific understanding and knowledge gaps, highlighting directions for future research and recognizing the information needs of policymakers and stakeholders. Expected final online publication date for the Annual Review of Environment and Resources, Volume 45 is October 19, 2020. Please see http://www.annualreviews.org/page/journal/pubdates for revised estimates.