Exposure of a clean gold surface to tetrahydrofuran (THF) under ambient conditions was observed to cause roughening of atomic step edges. This change was followed in situ using a scanning tunneling microscope during the exposure of a gold surface to a controlled stream of THF vapor. THF is a common solvent used in depositing molecules, self-assembled monolayers, and polymer films on surfaces, in electrochemistry, and in chemical reactions. Unlike other solvents, such as methanol, ethanol and diethyl ether, however, we found that THF itself has a profound effect on the surface morphology that needs to be taken into account when reporting on the interactions of solutes with a bold surface. At the same time, this finding may present new opportunities in catalysis or nanostructuring of surfaces.