The various toxic effects associated with inorganic arsenic (iAs) warrants that exposure sources be identified. This pilot study evaluated if greater seafood consumption from Vieques-Puerto Rico is associated with increased exposure to iAs. Nail, hair, and urine samples were used as biomarkers of iAs exposure in adult women and men from Vieques classified as high (n = 31) and low (n = 21) seafood consumers, who reported eating fish and/or shellfish ≥1 time per week and once per month or less, respectively. The sum of urinary iAs (As III + As V), monomethylarsonic acid (MA[V]), and dimethylarsinic acid (DMA[V]), denoted as SumAs, fluctuated from 3.3 µg/g Cr (1.2 μg/L) to 42.7 μg/g Cr (42 μg/L) (n = 52). Levels of As in nail samples (n = 49) varied from 0.04 to 0.82 μg/g dry weight (dw), whereas in hair (n = 49) As was only detected in 49 % of the samples with a maximum value of 0.95 μg/g dw. None of the biomarkers of exposure to As exceeded exposure reference values for urine (50 μg/g Cr or 50 μg/L), nails (1 μg/g), or hair (1 μg/g). However, median (10.0 μg/g Cr; 10.6 μg/L) and 95th percentile (31.9 μg/g Cr; 40.4 μg/L) of urinary SumAs were higher in Vieques samples than in the those from the general population of other countries. Among the three biomarkers of exposure, nail samples reflected better the exposure to iAs from seafood consumption with significantly higher average As concentrations in high (0.24 μg/g) than low (0.12 μg/g) seafood consumers. Multivariate results for As in nail samples (R (2) = 0.55, p < 0.0001) showed a positive association with fish consumption, particularly for men, with levels increasing with years of residency in Vieques.