In North Carolina, Odocoileus virginianus (White-tailed Deer) are the definitive natural hosts of Fascioloides magna (Giant Liver Fluke). Previous research identified the enzootic range of Giant Liver Fluke in North Carolina to be within the Tar River and Roanoke River Basins in Halifax and neighboring counties. Recent Giant Liver Fluke infections of Ovis aries (Domestic Sheep), Capra hircus (Domestic Goat), Lama glama (Llama), Vicugna pacos (Alpaca), and Bos taurus (Cattle) outside the historic enzootic range prompted us to investigate the current range of Giant Liver Fluke in North Carolina. From September 2014 to January 2015, we examined livers from hunter-harvested White-tailed Deer within 16 North Carolina counties. We detected Giant Liver Fluke in livers from 5 counties, with an overall prevalence of 10.3%. Besides reporting the first Giant Liver Fluke infections of livestock in North Carolina, we documented new geographic localities (Cabarrus, Franklin, Mecklenburg, Union, Wake, and Washington counties) for Giant Liver Fluke. An increased impact on North Carolina livestock is likely with the possible range expansion of Giant Liver Fluke, which may be related to the increase in populations of White-tailed Deer.