Polychlorinated biphenyls (PCBs), chlorinated pesticides (i.e., dichlorodiphenyltrichloroethane (DDT) and its metabolites, chlordanes (CHLs), dieldrin, hexachlorobenzene (HCB), and mirex), polybrominated diphenyl ethers (PBDEs), perfluorinated chemicals (PFCs), and polyaromatic hydrocarbons (PAHs) were measured in blubber biopsy samples collected from 139 wild bottlenose dolphins (Tursiops truncatus) during 2003–2005 in Charleston (CHS), SC and the Indian River Lagoon (IRL), FL. Dolphins accumulated a similar suite of contaminants with ∑PCB dominating (CHS 64%, IRL 72%), followed by ∑DDT (CHS 20%, IRL 17%), ∑CHLs (CHS 7%; IRL 7%), ∑PBDE (CHS 4%, IRL 2%), PAH at 2%, and dieldrin, PFCs and mirex each 1% or less. Together ∑PCB and ∑DDT concentrations contributed ∼87% of the total POCs measured in blubber of adult males. ∑PCBs in adult male dolphins exceed the established PCB threshold of 17mg/kg by a 5-fold order of magnitude with a 15-fold increase for many animals; 88% of the dolphins exceed this threshold. For male dolphins, CHS (93,980ng/g lipid) had a higher ∑PCBs geomean compared to the IRL (79,752ng/g lipid) although not statistically different. In adult males, the PBDE geometric mean concentration was significantly higher in CHS (5920ng/g lipid) than the IRL (1487ng/g). Blubber ∑PFCs concentrations were significantly higher in CHS dolphins. In addition to differences in concentration of PCB congeners, ∑PBDE, TEQ, ∑CHLs, mirex, dieldrin, and the ratios ∑DDE/∑DDT and trans-nonachlor/cis-nonachlor were the most informative for discriminating contaminant loads in these two dolphin populations. Collectively, the current ∑PCB, ∑DDT, and ∑PBDEs blubber concentrations found in CHS dolphins are among the highest reported values in marine mammals. Both dolphin populations, particularly those in CHS, carry a suite of organic chemicals at or above the level where adverse effects have been reported in wildlife, humans, and laboratory animals warranting further examination of the potential adverse effects of these exposures.