Pollution Probe was founded in 1969 by a group of students and faculty at the University of Toronto out of a desire to address environmental issues. The group initially focused on air pollution and only the Ontario area, but gradually expanded to also focus upon other forms of environmental pollutionover time, and also nationwide concerns. According to the organization's history, they worked on getting restrictions on the use of DDT enacted in 1969, and later a ban throughout Canada. In 1970, they pushed for legislation to limit phosphates in detergents. In 1973, they helped initiate recycling programs in Ontario, and in 1979 they helped push for legislation to restrict emissions that cause acid rain. In 1988, they helped to get regulations passed to remove lead from gasoline, and in 1993, they launched an annual "Clean Air Commute" campaign to increase public awareness about transportation options that could help improve air quality, and by 1998 they achieved the passage of mandatory vehicle emission testing in Ontario. In 2004, Pollution Probe helped to obtain further regulations in Ontario to reduce metal smelter facility emissions that can cause acid rain. In 2010, the organization helped to persuade the legislature to enact regulations to limit car and truck greenhouse gas emissions. In 2013, the organization collaborated with five power utilities to launch the Electric Mobility Adoption and Prediction project. In 2016, Pollution Probe and Plug’n Drive issued a report with recommendations intended to increase sales and use of electric vehicles. In 2017, Pollution Probe was appointed one of the positions on an advisory group for developing a plan for getting more zero-emission vehicles in use. In 2019, Pollution Probe partnered with the Royal Bank of Canada to produce a report on watershed planning in the Great Lakes ecosystem. The report used data science to analysis the ecosystem's functions and determine future actions to improve its health.
In 2016, The First Green Wave, a book about the beginning of the environmental movement in Ontario, authored by Ryan O'Connor, won the Ontario Historical Society's J.J. Talman Award for being the best book on Ontario's social, economic, political or cultural history, published in the past three years. The book focused heavily upon the history of Pollution Probe.