Concentrations of several congeners and classes of organohalogen contaminants (OHCs) and/or their metabolites, namely organochlorine pesticides (OCs), polychlorinated biphenyls (PCBs), hydroxylated-PCBs (OH-PCBs), methylsulfonyl-PCBs (MeSO(2)-PCBs), polybrominated diphenyl ether (PBDE) flame retardants, and OH-PBDEs, were measured in cerebrospinal fluid (CSF) of short-beaked common dolphins (n = 2), Atlantic white-sided dolphins (n = 8), and gray seal (n = 1) from the western North Atlantic. In three Atlantic white-sided dolphins, cerebellum gray matter (GM) was also analyzed. The levels of OCs, PCBs, MeSO(2)-PCBs, PBDEs, and OH-PBDEs in cerebellum GM were higher than the concentrations in CSF. 4-OH-2,3,3',4',5-pentachlorobiphenyl (4-OH-CB107) was the only detectable OH-PCB congener present in CSF. The sum (Sigma) OH-PCBs/Sigma PCB concentration ratio in CSF was approximately two to three orders of magnitude greater than the ratio in cerebellum GM for dolphins.