After spending three years at Augustana College, Tsui graduated Phi Beta Kappa in 1961 as the only student of Chinese descent in his college. Tsui continued his study in physics at the University of Chicago, from where he received his Ph.D. in physics in 1967 after completing a doctoral dissertation, titled "de Haas-van Alphen effect and electronic band structure of nickel", under the supervision of Royal Stark. He remarked that due to the influence of prominent Chinese theoretical physicists and Nobel laureates C. N. Yang and T. D. Lee, both of whom studied at the University of Chicago, he had always knew that he wanted to pursue graduate studies in physics at the institution.