Vapor-liquid equilibrium (VLE) data for allyl alcohol + water and allyl alcohol + benzene systems have been determined at 101.3 kPa using a circulation VLE still. The experimental data were checked both with the Herington consistency test and van Ness consistency test methods, which indicates that the experimental data satisfy the examination of the thermodynamic consistency. Moreover, all equilibrium data were correlated with Wilson, nonrandom two-liquid (NRTL), and universal quasichemical (UNIQUAC) activity coefficient models to obtain the binary interaction parameters of these models using Aspen Plus commercial software. The results show that the two systems forms a minimum temperature binary azeotrope.