Environmental specimen banks (ESBs) have been a fundamental tool for many nations to monitor contaminant temporal and spatial trends, study fate and transport, and assess the severity and risks of pollution. The specimens archived in ESBs are among the longest time-series, most geographically robust, and highest integrity samples available for performing environmental research. Mercury (Hg) remains one of the world's most ubiquitous environmental contaminants, and ESBs have played a prominent role in Hg research. Historically this has involved measuring concentrations of Hg species in various environmental matrices, but the emerging field of Hg stable isotope research provides a new analytical approach that can augment these traditional techniques. Signatures of Hg isotope fractionation have been effectively used for source apportionment and for elucidating Hg biogeochemical cycling. As the research surrounding Hg stable isotopes continues to mature, ESBs can play a useful role in analytical quality control, provide a robust and economical sample archive to expand and diversify the inventory of Hg isotope measurements, and be used to develop and test hypotheses to evaluate whether broadly prevailing paradigms are supported. Samples archived in ESBs are available for request by external collaborators in order to perform high impact research, and should be utilized more effectively to address emerging global environmental concerns.