Steller sea lion (Eumetopias jubatus) tissue mercury concentrations increasingly above thresholds of concern occur in regions of Alaska where lack of population recovery is noted. Selenium-monomethylmercury interactions may mitigate toxicosis but may also result in functional selenium deficiency, impacting essential selenium-dependent processes. Physiologically driven differences in tissue concentrations (organotropism) of total mercury ([THg]), total selenium ([TSe]), and monomethylmercury ([MeHg + ]) confound interpretation for various age cohorts. Archived tissues from Alaska Steller sea lions (2002)(2003)(2004)(2005)(2006)(2007)(2008)(2009)(2010)(2011)(2012)(2013)(2014)(2015)(2016) were used to compare [THg], [MeHg + ], and [TSe] across age cohorts and tissue types. Liver [THg] ranged from 0.05 to 63.7 µg/g. Fetal and pup livers had significantly lower [THg] and [TSe], higher percentage MeHg + , and greater range of molar TSe:THg than subadult and adult livers. Molar Se:MeHg + ratios, including Se in excess of nonmethylmercury, were dependent on [MeHg + ] in fetuses and pups. While [THg] varied significantly by muscle type (heart vs. skeletal) and anatomical location, concentrations were strongly correlated. Biomagnification and/or bioaccumulation of THg in liver of older animals confounded comparison with other tissues; however, in fetal and pup liver [THg] correlated with other tissues. In contrast, liver [MeHg + ] correlated with other tissues across all age classes. Fetal and pup tissues, which reflect in utero exposure and are subject to limited bioaccumulation, are ideal for assessing mercury exposure related to dam diet, including intertissue comparison, and represent key cohorts of concern. Evaluating [MeHg + ] and [TSe] in tissues from multiple age cohorts allows better intertissue comparison, providing insight into time courses, routes of exposure, and potential for adverse effects.