The isobaric binary vapor-liquid equilibrium (VLE) data for the mixture of acetophenone (ACP) and 2-phenylethanol (PEA) is generated at atmospheric and sub-atmospheric conditions in a modified Rose-type equilibrium still. Fredenslund test and Redlich-Kister area test methods were used to verify the consistency of the measured VLE experimental data. Furthermore, the measured experimental data is correlated by the non-random two-liquid (NRTL), universal quasi-chemical (UNIQUAC), and Wilson thermodynamic models, and the binary interaction parameters for the three models were estimated using a maximum likelihood objective function and Britt-Luecke algorithm. The estimation was found to be considerably good for all three activity coefficient models.