The vapor−liquid equilibrium data of the three binary systems, including the components of cumene, t-butylbenzene, and sec-butylbenzene, were determined at 101.3 kPa in this paper. The systems did not exhibit azeotropic behavior under the experimental conditions. The Fredenslund test, the Redlich−Kister area test, and Wisniak's L-W test checked the thermodynamic consistency of the vapor−liquid equilibrium data. The experimental data were correlated by nonrandom two-liquid, Wilson, and universal quasi-chemical activity coefficient models, and their respective binary interaction parameters were obtained correspondingly. The maximum absolute deviation, root-mean-square deviation, and average absolute deviation between experimental data and computed values by thermodynamic models were calculated as well. It showed that all three models could fit the experimental data well. This study can help in designing the distillation process in industrial applications.