Although the Turtle/Brunswick River Estuary (TBRE) in coastal Georgia (USA) is severely contaminated by persistent organochlorine pollutants (POPs), little information regarding POPs in higher-trophic-level biota in this system is available. In the present study, polychlorinated biphenyls (PCBs), organochlorine pesticides (OCPs; including DDTs, chlordanes, and mirex), and chlorinated monoterpenes (toxaphene) were measured using gas chromatography with electron-capture detection and gas chromatography with electron-capture negative ion mass spectrometry (GC-ECNI-MS) in blubber of free-ranging and stranded bottlenose dolphins (Tursiops truncatus). Mean total PCBs (78.6 ± 32.4 μg/g lipid) and toxaphene (11.7 ± 9.3 μg/g lipid) were significantly higher in dolphins sampled in the TBRE than in dolphins stranded near Savannah (GA, USA) 80 to 100 km to the north. Levels of OCPs were several-fold lower than levels of PCBs; moreover, PCBs comprised 81 and 67% of the total POP burden in TBRE and non-TBRE dolphins, respectively. Analyses with GC-ECNI-MS revealed that 2,2,5-endo,6-exo,8,8,9,10-octachlorobornane (P-42a), a major component in technical toxaphene and a major residue congener in local estuarine fish species, was the most abundant chlorobornane in both sets of blubber samples. Mean total POP concentrations (sum of PCBs, OCPs, and toxaphene) approached 100 μg/g lipid for the TBRE animals, well above published total PCB thresholds at which immunosuppresion and/or reproductive anomalies are thought to occur. These results indicate extended utilization of the highly contaminated TBRE as habitat for a group of coastal estuarine dolphins, and they further suggest that these animals may be at risk because of elevated POP concentrations.