About half of the world's population now lives in urban areas because of the opportunity for a better quality of life. Many of these urban centers are expanding rapidly, leading to the growth of megacities, which are defined as metropolitan areas with populations exceeding 10 million inhabitants. These concentrations of people and activity are exerting increasing stress on the natural environment, with impacts at urban, regional and global levels. In recent decades, air pollution has become one of the most important problems of megacities. Initially, the main air pollutants of concern were sulfur compounds, which were generated mostly by burning coal. Today, photochemical smog--induced primarily from traffic, but also from industrial activities, power generation, and solvents--has become the main source of concern for air quality, while sulfur is still a major problem in many cities of the developing world. Air pollution has serious impacts on public health, causes urban and regional haze, and has the potential to contribute significantly to climate change. Yet, with appropriate planning, megacities can efficiently address their air quality problems through measures such as application of new emission control technologies and development of mass transit systems. This review is focused on nine urban centers, chosen as case studies to assess air quality from distinct perspectives: from cities in the industrialized nations to cities in the developing world. While each city--its problems, resources, and outlook--is unique, the need for a holistic approach to the complex environmental problems is the same. There is no single strategy in reducing air pollution in megacities; a mix of policy measures will be needed to improve air quality. Experience shows that strong political will coupled with public dialog is essential to effectively implement the regulations required to address air quality problems.