The influence of fluoride emissions from a modern aluminum smelter on concentrations of skeletal fluoride and dental fluorosis in a resident population of white-tailed deer was studied. The smelter was located on Mount Holly Plantation in South Carolina, and concentrations of skeletal fluoride in the deer collected at Mount Holly increased approximately five-fold 3 yr after the operation began. Increases in skeletal fluoride of less than two-fold were observed in deer obtained from Medway Plantation which has its nearest boundary 1.6 km from the smelter site. No dental fluorosis was observed in deer collected at Medway Plantation, but mild dental fluorosis was observed in a significant number of deer collected at Mount Holly Plantation. The dental fluorosis that was observed was not associated with incisor wear or with fluoride-induced molar wear. Osteofluorosis of mandibles or metacarpals was not observed in any of the deer obtained from either plantation. The data obtained from this study indicated that the presence of a modern aluminum smelter caused a detectable increase in concentration of skeletal fluoride in the resident population of white-tailed deer, but that no adverse health effects were seen.