After continued recruitment efforts by Venable, the president of the University of North Carolina at Chapel Hill (UNC) at the time, Herty finally accepted a long-offered appointment as the head of that school's chemistry department in January 1905 and served as the Smith Professor of Applied Chemistry, officially beginning his duties in July of that year. In 1908, Herty was appointed the dean of UNC's School of Applied Sciences and served in that position until 1911. During his tenure at UNC, Herty continued to receive numerous job offers from groups including UGA as the Chair of Forestry, the United States Department of Agriculture Bureau of Soils, the Forest Products Laboratory, the University of Virginia, and the Massachusetts Institute of Technology; however, Herty remained at UNC.