Fur is a common biomarker of environmental mercury (Hg) exposure. Further, there are well-established relationships between total mercury (THg) in fur and organs. However, these models assumed that THg is uniformly distributed across the fur in a pelt. In this study, we assess the distribution of THg and methylmercury (MeHg) across the pelts of four river otters (Lontra canadensis) . THg concentrations were measured in the topcoat (n = 95) and undercoat fur (n = 95). MeHg was measured in a subset of these samples (n = 10). Patterns of THg and MeHg were explored using cluster analyses and ANOVAs. Significant differences existed between THg in topcoat and undercoat and between anatomical region (head/body/tail/legs) and fur regions (dorsal/ventral/furline). The cluster analysis showed significant THg clusters in undercoat fur and to a lesser extent topcoat fur. Further, the error rate for predicting internal THg is lowest in the forebody region of the topcoat, thus, making this the optimal region to sample for biomonitoring. Fur samples taken outside of this region could result in prediction error as high as 140% when estimating internal organ THg. The ratio of MeHg in THg in topcoat fur was measured at 95.7 ± 3.4% indicating THg concentrations can be used to assess MeHg exposure.