Olmsted was born June 18, 1791 in East Hartford, Connecticut. In 1813, he graduated from Yale College, where he acted as college tutor from 1815 to 1817. In the latter year, he was appointed to the chair of chemistry, mineralogy and geology in the University of North Carolina at Chapel Hill. A gold rush in North Carolina spurred the state legislature to sponsor the first state geological survey that was ever attempted in the United States. Olmsted traveled by horseback across the state collecting minerals and fossils, publishing his geological map in 1825.