North American pollutant release and transfer registries have been continuously developing with an eye to understanding source/receptor relationships and ensuring that the polluter-paid principle is applied to the appropriate parties. The potential contribution of mercury to the Great Lakes Basin arising from the rerelease of historic mercury pollution from contaminated aquatic and terrestrial media is poorly understood and the subject of concern. Although a considerable amount of data may be available on the atmospheric component of mercury releases to the Basin, further inventory work is needed to quantify the rerelease of the historic mercury. Much of the related existing inventory information is either not derived from direct measurement or not bounded by a mass-balance accounting. Critical to this determination is an increased confidence in the inventories of mercury from past and current practices. This may be enhanced through comprehensive and thorough surveys of contributions from specific products and their life-cycle assessments. An even greater challenge is to determine the bioavailability of the mercury emanating from land-based sources and from aquatic media. This paper describes the interplay among the sources and receptors of mercury and provides a quantitative assessment of current Canadian contributions of mercury as a contaminant to the Great Lakes. Recommendations for improved assessments are provided.