The distribution of perfluoroalkyl compounds (PFCs) in the environment is well documented with higher concentrations observed in wildlife located in industrial and urban areas. This study examined the distribution of PFCs in relation to land use using blood samples collected from bottlenose dolphins during capture-release health assessment surveys conducted in Charleston, SC. The study area was partitioned into three subareas (ACW, CHS, and SRE) based upon habitat and land use characteristics. The ACW and CHS subareas are characterized by high degrees of industrial and urban land uses, while the SRE subarea is more residential and characterized by a lower degree of developed land use. Long-term monitoring data from photo-identification surveys were used to group bottlenose dolphins based on their proportions of sightings in the different subareas. Dolphins affiliated with both the ACW and CHS subareas were observed to have significantly higher mean plasma concentrations of perfluorooctane sulfonate (PFOS), perfluorodecanoic acid (PFDA) and perfluoroundecanoic acid (PFUnA) than those affiliated with the SRE subarea. Dolphins affiliated with the ACW subarea were found to have a significantly higher mean plasma concentration of PFUnA than those affiliated with the CHS subarea. Further examination of the distribution of the PFCs revealed positive correlations with developed land uses and negative correlations with wetland/marsh land cover. A positive correlation was also observed between PFUnA and agricultural land use. The variability and scale of the observed contaminant burdens have important implications for the conservation and management of living marine resources and illustrates the importance of long-term monitoring of free-ranging wildlife species.