The isobaric vaporliquid equilibrium data for the two binary systems of (3-methyl-1-butanol + 1,4-butanediol, hexylene glycol + 1,4-butanediol) at p = 40.0, 60.0, and 80.0 kPa were obtained by a improved Rose equilibrium still. The thermodynamic consistency of the VLE (vaporliquid equilibrium) data was checked via the methods of the Herington area test and the Van Ness point test. In addition, the nonrandom two-liquid (NRTL), Wilson, and universal quasichemical (UNIQUAC) activity coefficient models were adopted to correlate the VLE data. The calculated values of the models mentioned above showed good agreements with the measured data.