Surveillance data collected over the past 150 years are compiled and analyzed to identify chloride trends in the Laurentian Great Lakes. These data indicate that chloride levels started rising in the mid-19th century and began accelerating in the early twentieth century. Lake Superior's and Lake Michigan's concentrations have continued to increase steadily and currently stand at their maximum recorded levels. In contrast, lakes Huron, Erie and Ontario reached peak levels between 1965 and 1975, but then began to decline. However, recent data indicate that the chloride concentrations in these lakes are now increasing again. Because loading data are not readily available, a mass-balance model is employed to estimate the chloride inputs required to account for the concentration trends. This inverse analysis yields computed load reductions that are consistent with reported industrial load reductions during the last three decades of the 20th century. Hence, it appears that the improvements were for the most part attributable to industrial controls. The model is also used to predict that if loads are held fixed at 2006 levels, concentrations in all lakes will continue to increase with the most dramatic rise occurring in Lake Michigan which will ultimately approach the level of Lake Erie.