The global dispersal of forests and soils has been proposed as a cause for the Late Devonian mass extinctions of marine organisms, but detailed spatiotemporal records of forests and soils at that time remain lacking. We present data from microscopic and geochemical analyses of the Upper Devonian Chattanooga Shale (Famennian Stage). Plant residues (microfossils, vitrinite and inertinite) and biomarkers derived from terrestrial plants and wildfire occur throughout the stratigraphic section, suggesting widespread forest in the southern Appalachian Basin, a region with no macro plant fossil record during the Famennian. Inorganic geochemical results, as shown by increasing values of SiO2/Al2O3, Ti/Al, Zr/Al, and the Chemical Index of Alteration (CIA) upon time sequence, suggest enhanced continental weathering that may be attributed to the invasion of barren lands by rooted land plants. Our geochemical data collectively provide the oldest evidence of the influences of land plants from the southernmost Appalachian Basin. Our synthesis of vascular plant fossil record shows a more rapid process of afforestation and pedogenesis across south-central Euramerica during the Frasnian and Famennian than previously documented. Together, these results lead us to propose a new hypothesis that global floral dispersal had progressed southward along the Acadian landmass rapidly during the Late Devonian.