Water striders (Hemiptera: Gerridae) have been considered as a potential sentinel for mercury (Hg) contamination of freshwater ecosystems, yet little is known about factors that control Hg concentrations in this invertebrate. Striders were collected from 80 streams and rivers in New Brunswick, Canada, in August and September of 2004 through 2007 to assess the influence of factors such as diet, water chemistry, and proximity to point sources on Hg concentrations in this organism. Higher than average Hg concentrations were observed in the southwest and Grand Lake regions of the province, the latter being the location of a coal-fired power plant that is a source of Hg (approximately 100 kg annually), with elevated Hg concentrations in the lichen Old Man's Beard (Usnea spp.) in its immediate vicinity. Across all streams, pH and total organic carbon of water were relatively weak predictors of strider Hg concentrations. Female striders that were larger in body size than males had significantly lower Hg concentrations within sites, suggestive of growth dilution. There was no relationship between percent aquatic carbon in the diet and Hg concentrations in striders. For those striders feeding solely on terrestrial carbon, Hg concentrations were higher in animals occupying a higher trophic level. Mercury concentrations were highly variable in striders collected monthly over two growing seasons, suggesting short-term changes in Hg availability. These measurements highlight the importance of considering both deposition and postdepositional processes in assessing Hg bioaccumulation in this species. They also suggest that striders may be more appropriate as a terrestrial rather than an aquatic Hg sentinel, underscoring the importance of understanding the origin of food for organisms used in contaminant studies.