Mosses are a major component of the tundra flora in the Canadian Arctic, yet their use in arctic contaminant research is lacking. Biomonitoring of atmospheric heavy metal deposition using mosses has been extensively employed in Europe, providing a higher sampling density than precipitation monitoring. Temporal, spatial, and habitat gradients of concentrations and enrichment factors of As, Cd, Cr, Cu, Ni, Zn, and Pb (and its stable isotopes) in mosses from Ellesmere Island are examined. Anthropogenically influenced concentrations of As, Cr, Cu, Ni, and Zn in samples collected in 2007 were observed. Concentrations of heavy metals in hydric taxa were larger than those observed in xeric or mesic taxa, though non-significant. Generally, heavy metal concentrations decreased from 1983 to 2007 in a single high arctic locality, though non-significant. Pb-isotope ratios were radiogenic and characteristic of the High Arctic Islands. Trends in high arctic moss data corresponded with environmental proxies such as glacial ice cores, lake sediments, and atmospheric aerosols illustrating the usefulness of bryophytes as biomonitors. This paper outlines the utility of using mosses as biomonitors of heavy metal depositions in the Canadian High Arctic.