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Biomonitoring programs for persistent, bioaccumulative, and/or toxic chemicals of concern in fish tissues have been operated by the governments of Canada and the United States in the Great Lakes since the 1970's. The objectives of these programs are to assess concentrations of harmful chemicals in whole body top predator fish as an indicator of ecosystem health and to infer potential harm to fish and fish consuming wildlife in the Great Lakes Basin. Chemicals of interest are selected based upon national and binational commitments, risk assessment, and regulation, and include a wide range of compounds. This review summarizes all available data generated by Environment Canada and the United States Environmental Protection Agency for chemicals measured in whole body homogenates of Lake Trout (Salvelinus namaycush) and Walleye (Sander vitreus) for the time period spanning 2008 to 2012 from each of the five Great Lakes. The summary shows that concentrations of legacy compounds, such as, POPs listed in the Stockholm Convention and mercury continue to dominate the chemical burden of Great Lakes fish. This assessment, and others like it, can guide the creation of environmental quality targets where they are lacking, optimize chemical lists for monitoring, and prioritize chemicals of concern under agreements such as the Great Lakes Water Quality Agreement and the Stockholm Convention. Crown Copyright (C) 2015 Published by Elsevier Ltd.