Smith was born on September 25, 1916, in Long Beach, California, and he grew up in Long Beach and Fontana, California. He attended Pomona College, graduating in 1938, and was a member of the Phi Beta Kappa honors society. While as a student at Pomona, Smith authored two papers with his chemistry professor, Wesley G. Leighton. After leaving Pomona, Smith went to Stanford University to work under Leighton's brother Philip A. Leighton and was awarded an M.A. and Ph.D. in 1940 and 1942 respectively.