Vapor-liquid equilibria (VLE) data for the toluene + ethanol and toluene + isopropanol binary systems have been measured at (101.3, 121.3, 161.3, and 201.3) kPa using a VLE recirculating still. The experimental data were checked with the Herington method, which showed thermodynamic consistency. The experimental VLE data were correlated with Wilson, nonrandom two-liquid (NRTL), and universal quasichemical (UNIQUAC) activity coefficient models. The results show that the calculated values of the vapor-phase mole fraction and boiling temperature by the Wilson, NRTL, and UNIQUAC models agree well with the experimental data. Furthermore, azeotropic VLE behaviors can be observed from the experimental data.