Charles P. Smyth begins the interview by naming the many scientists in his family and discussing his undergraduate education at Princeton, with descriptions of the curriculum, faculty, and facilities. He then describes his tenure at the National Bureau of Standards and the Chemical Warfare Service, where he worked on electroplating and poison gas during the First World War. Smyth continues with a discussion of his Ph.D. training at Harvard, where his thesis examined thallium amalgams. He then describes his return to Princeton as an instructor, his early teaching and students, and the options he considered for research projects. His work on dipole moment lead to an important discovery about benzene ring structure that proved correct the Kekul ̌model. He then discusses the funding situation at Princeton and his first visits to Europe, where he meets Peter Debye, Karl Bonhf̲fer and James Franck. Smyth next discusses department colloquia at Princeton, attempts to recruit Debye and Enrico Fermi to Princeton, and changes in the chemical field during the 1920s and 1930s, including the emergence of chemical physics. The interview ends with a discussion of Smyth's work on deuterium and the Manhattan Project. In the appendix, "Scientist in a Jeep," Smyth narrates a detailed account of his work in the U.S., France and Germany with the ALSOS Mission, which investigated Nazi Germany's scientific capabilities at the end of the Second World War.