In both the North Sea and the Açu Port (Brazil) coastal areas, high As concentrations were observed in water, soil and sediments. Therefore, the impact of this contamination on fish and shellfish species bought from local fishermen was studied. Total As was assessed by ICP-MS while toxic As was assessed by ICPMS-HPLC and HG-AFS. Several fish species had average Total As concentrations above 1 mg g−1, but the highest concentrations were found in less spotted dogfish, lemon sole and whelks from the North Sea. Toxic As fractions were high in scallops but rarely exceeded 2% in other species. Considering consumption of 150 g, only 3 samples exceeded the total daily intake. Using mean toxic As concentrations for each species, lifetime cancer risk values at the actual global seafood consumption rate of 54 g/day are above 10−4 for whelks, scallops, dogfish, ray and lemon sole.