The Big Ivy section of Pisgah National Forest in North Carolina was surveyed to produce a baseline bryophyte species list. Big Ivy is a minimally disturbed 5700-hectare mature forested headwaters tract in the heart of the botanically rich Southern Appalachian Mountains and has not previously been surveyed for bryophytes. From twenty sites representing common and unique habitats, roughly 5000 specimens were examined and 735 were retained. Two hundred sixty-six species were identified, including 182 mosses, 83 liverworts, and one hornwort, representing 38% of the 692 bryophyte taxa estimated to occur in North Carolina. Twenty-seven species are listed as rare in the state. Four are new or recent finds for the southeastern United States: Fissidens closteri, Ptychomitrium serratum, Schistidium papillosum, and Zygodon viridissimus. Habitats notable for exceptional diversity and rare species include montane alluvial forest, fog-prone high ridges, rocky tumbling streams, and a 20 m waterfall over a wet rockhouse.