Mercury exposure through the consumption of fish and shellfish represents a significant public health concern in the United States. Recent research has demonstrated higher seafood consumption and subsequent increased risk of methylmercury exposure among subpopulations living in coastal areas. The identification of high concentrations of total mercury in blood and skin among resident Atlantic bottlenose dolphins (Tursiops truncatus) in the Indian River Lagoon (IRL), a coastal estuary in Florida, alerted us to a potential public health hazard in the contiguous human population. Therefore, we analyzed hair mercury concentrations of residents living along the IRL and ascertained their sources and patterns of seafood consumption. The total mean mercury concentration for 135 residents was 1.53 ± 1.89 µg/g. The concentration of hair mercury among males (2.02 ± 2.38 µg/g) was significantly higher than that for females (0.96 ± 0.74 µg/g) (p < 0.01). Log transformed hair mercury concentration was significantly associated with the frequency of total seafood consumption (p < 0.01). Individuals who reported consuming seafood once a day or more were 3.71 (95% CI 0.84-16.38) times more likely to have a total hair mercury concentration over 1.0 µg/g, which corresponds approximately to the U.S. EPA reference dose, compared to those who consumed seafood once a week or less. Hair mercury concentration was also significantly higher among individuals who obtained all or most of their seafood from local recreational sources (p < 0.01). The elevated human mercury concentrations mirror the elevated concentrations observed in resident dolphins in the same geographical region. The current study is one of the first to apply the concept of a sentinel animal to a contiguous human population.