Mercury (Hg) concentration trends in top predator fish (lake trout and walleye) of the Great Lakes (GL) from 2004 to 2015 were determined by Kendall-Theil robust regression with a cluster-based age normalization method to control for the effect of changes in lake trophic status. When data from the GLs (except Lake Erie) are combined, a significant decreasing trend in the lake trout Hg concentrations was found between 2004 and 2015 with an annual decrease of 4.1% per year, consistent with the decline in regional atmospheric Hg emissions and water Hg concentrations. However, a breakpoint was detected with a significant decreasing slope (-8.1% per year) before the breakpoint (2010), and no trend after the breakpoint. When the lakes are examined individually, Lakes Superior and Huron, which are dominated by atmospheric Hg inputs and are more likely than the lower lakes to respond to declining emissions from areas surrounding the GL, have significant decreasing trends with rates between 5.2 and 7.8% per year from 2004 to 2015. These declining trends appear to be driven by decreasing regional atmospheric Hg emissions although they may be partly counterbalanced by other factors, including increasing local emissions, food web changes, eutrophication, and responses to global climate change. Lakes Michigan, Erie and Ontario may have been more impacted by these other factors and their trends changed from decreasing to non-decreasing or increasing in recent years.

Concentration patterns and temporal trends of legacy persistent, bioaccumulative and toxic (PBT) contaminants were determined using the Great Lake Fish Monitoring and Surveillance Program (GLFMSP) top predator fish data from 1999 to 2014 and applying Kendall-Theil robust regression after cluster-based age normalization. For most Great Lakes sites, significant decreasing concentration trends ranging from −4.1% to −21.6% per year (with the only exception being mirex in Lake Erie walleye) were found for PBTs including polychlorinated biphenyls (PCBs), dichlorodiphenyl-trichlorethane (DDTs), dieldrin, endrin, chlordane, oxychlordane, nonachlor, mirex, and hexachlorobenzene (HCB) reflecting the successful historical and ongoing reduction of fugitive releases and remediation efforts in the U.S. and Canada including physical removal (dredging) coupled with sediment sequestration. Generally, lower concentrations and faster decreasing trends are observed in western/northern sampling sites compared to eastern/southern sites as the former sites are generally more remote from population centers and industrial activities. PCBs, which can be released from ongoing sources, have the highest concentration, the second slowest decreasing trend, and increasing mass fractions of the contaminants studied suggesting that they will continue to be the legacy contaminant of greatest concern into the future.