The bioaccessible concentration and speciation of arsenic (soluble in a gastrointestinal medium and available for absorption into the bloodstream) were determined in softshell clams (Mya arenaria), harvested by local residents until 2005, and in seaweed (Fucus sp.) from an arsenic-contaminated marine site in Seal Harbour, Nova Scotia, Canada. Bioaccessibility extractions to simulate the human gastrointestinal environment (pH 1.5 and glycine for 1h followed by pancreatin, bile extract and pH adjustment to 7 for an additional 4h) and speciation of arsenic in extracts (HPLC-HG-AAS to target inorganic arsenic species) and whole samples (XANES) were carried out. Total arsenic for the clams from the contaminated area ranged from 218 to 228 ppm wet weight, with a bioaccessible fraction of 34-46%, and the major bioaccessible species of arsenic were inorganic. The seaweed from the contaminated area contained 27-43 ppm wet weight total arsenic, with the bioaccessible fraction ranging from 63% to 81%, and inorganic arsenic was also predominant. The predominantly inorganic nature of arsenic in the whole samples was confirmed by XANES. In concurrence with the closure of the area for clam harvesting, the clams and seaweed from Seal Harbour should probably not be used for human consumption.