Rowland held academic posts at Princeton University (1952–56) and at the University of Kansas (1956–64) before becoming a professor of chemistry at the University of California, Irvine, in 1964. At Irvine in the early 1970s he began working with Mario J. Molina. Rowland was elected to the National Academy of Sciences in 1978 and served as a president of American Association for the Advancement of Science (AAAS) in 1993. His best-known work was the discovery that chlorofluorocarbons contribute to ozone depletion. Rowland theorized that man made organic compound gases will decompose as a result of solar radiation in the stratosphere, releasing atoms of chlorine which react with oxygen (ozone) to form chlorine monoxide, and that they are individually able to destroy large numbers of ozone molecules. It was obvious that Rowland had a good idea of what was occurring at higher altitudes when he stated "...I knew that such a molecule could not remain inert in the atmosphere forever, if only because solar photochemistry at high altitudes would break it down". Rowlands research, first published in Nature' magazine in 1974, initiated a scientific investigation of the problem. In 1978, a first ban on CFC-based aerosols in spray cans was issued in the United States. The actual production did however not stop and was soon on the old levels. It took till the 1980s to allow for a global regulation policy.
Rowland performed many measurements of the atmosphere. One experiment included collecting air samples at various cities and locations around the globe to determine CClF North-South mixing. By measuring the concentrations at different latitudes, Rowland was able to see that CClF was mixing between hemispheres quite rapidly. The same measurement was repeated 8 years later, and the results showed a steady increase in CClF concentrations. Rowland's work also showed how the density of the ozone layer varied by season increasing in November and decreasing until April where it levels out for the summer only to increase in November. Data gained throughout successive years showed that although the pattern was consistent, the overall ozone levels were dropping. Rowland and his colleagues interacted both with the public and the political side and suggested various solutions, which allowed to step wise reduce the CFC impact. CFC emissions were regulated first within Canada, the United States, Sweden and Norway. In the 1980s, the Vienna Agreement and the Montreal Protocol allowed for global regulation.