The 21st century Olympic Agenda aims to align itself with the concept of sustainable development and has driven improved environmental quality in host cities, such as the Green Games in Sydney 2000 and the planned Beijing 2008 Games and in London 2012 as the Low Carbon Games. Air quality has long been a concern of Olympic mega-cities, although the air quality plans and strategies have often seemed short-lived and unsustainable in the long term. We have explored air quality data and air pollution control from seven Olympic cities: Mexico City, Los Angeles, Atlanta, Sydney and Athens and also Beijing and London which will host Olympic Games in near future. The study shows that despite a high altitude and air pollution problems, Mexico City had no clear environmental policy in place for the 1968 games. The characteristic smog of Los Angeles raised concerns about athletic performance at the Olympic Games of 1984, but there were limited efforts to tackle the ozone concentration during these games. The 1996 Atlanta Games represents a case where temporary public transport changes were used as a tactic to reduce air pollution. In Sydney a well planned sustainable strategy reduced air pollutants and CO2 emissions in 2000, but Athens' long efforts to improve air quality for the 2004 games were not wholly effective. Even where strategies proved successful the improvements in air quality seem short-lived. Current host cities Beijing and London are developing emission reduction plans. These have clear air quality objectives and are well intentioned. However, the improvements may be too narrow and may not be sustainable in the long term. Our analysis looks at the origins of success and failure and how more coherent improvements might be achieved and what would promote sustainable plans for air quality management at future games. The study illustrates the feedback between air pollution science and policy awareness.