The levels of mercury (Hg) were examined in the leg muscle of the crab Grapsus grapsus from five sites on four islands within the Galápagos archipelago. Mercury values obtained using a Milestone DMA 80 evo direct mercury analyzer varied both within and among sites. Total mercury concentrations (mg kg−1 dry weight) ranged from the lowest at a protected location at Isabela Island (0.06 ± 0.02) to the highest at the San Cristóbal urban location (2.04 ± 0.069). Crabs from South Plaza Island also had surprisingly high levels of mercury with a mean of 1.2 ± 0.6. Values from urban sites at Isabela Island and Academy Bay, Santa Cruz, had intermediate values. When converted to wet weight, crabs from both San Cristóbal and South Plaza were within or above the levels (0.3–0.5 mg kg−1 wet weight set by various government agencies) considered potentially harmful to human health if ingested. A lesser number of both oysters and barnacles were also analyzed for mercury at South Plaza and Academy Bay, and while the values were lower compared to the crabs, they followed the same pattern of elevated levels at South Plaza compared to Academy Bay. It is unclear as to whether the mercury comes from natural sources, such as volcanism, or anthropogenic causes.