Long sediment cores (> 1 m) were collected from eight Precambrian Shield lakes in southern Ontario, Canada and analyzed for mercury (Hg), loss-on-ignition (LOI), and a suite of 36 other elements. Results indicated at least 100-fold variation in sediment Hg concentrations between lakes in close proximity (from 450 ppb), comparable to the variation reported for lakes across the whole of Canada. Strong areal correlations between Hg concentrations and LOI (r2=0.77), between Hg and other trace element concentrations (Pb, Zn, Cd, Sb, As, Br), and similarities in the vertical concentration profiles of Hg and LOI, all point to the importance of organic matter in the release, transport and redistribution of metals in watershed systems. The spatial pattern of Hg concentrations in deep, precolonial sediments (>20 cm) was found to mirror the pattern of Hg concentrations in modern surface sediments, an observation that was confirmed in a follow-up survey (r2= 0.85; n = 25 lakes), indicating that natural processes govern the unequal distribution of Hg among these lakes. Between-lake differences in surface sediment Hg concentrations normalized to organic carbon (Hg/C) were also reflected by Hg concentrations in small-mouth bass normalized to 35 cm length (R2=0.63; n= 15 lakes). The latter relationship suggests that small-mouth bass and lake sediment indicators provide mutually supportive information regarding Hg loading to the lacustrine environment from geological sources in the watershed system.