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In the relatively pristine ecosystem in Kejimkujik Park, Nova Scotia, methylmercury (MeHg) concentrations in loons, Gavia immer, are among the highest recorded anywhere in the world. This study investigated the influence of bedrock lithology on MeHg concentrations in wetlands. Twenty‐five different wetland field sites were sampled over four different bedrock lithologies; Kejimkujik monzogranite, black sulfidic slate, gray slate, and greywacke. Soil samples were analyzed for ethylmercury (EtHg), MeHg, total Hg, acid‐volatile sulfides (AVS), organic matter, and water content as well as the biological parameters, mercury methyltransferase (HgMT) activity, sulfate reduction rates, fatty acid methyl ester (FAME) composition, and acidity. Methylmercury concentrations in the wetlands were highly dependent (P< 0.08) on lithology with no significant difference between bogs, fens, and swamps. Methylmercury concentrations in wetland soils developed on Kejimkujik monzogranite averaged 900 ng kg−1compared with only 300 ng kg−1in wetland soils developed on black sulfidic slate. Fatty acid methyl ester composition was also lithologically dependent (P< 0.001) with biomarkers for Desulfobulbusspp. discriminating between sites containing high and low MeHg concentrations. Levels of MeHg in wetlands were predicted mainly (41% of the sum of squares) by HgMT activity that differed (P< 0.009) between wetlands, with activity in bogs almost three times that present in swamps. Wetland MeHg concentrations are highly dependent on the lithology on which they have developed for largely biological reasons.