The aim of this work was to measure and model high precision isothermal binary vapor liquid equilibrium (VLE) phase data for the pentan-2-one + propan-1-ol/butan-1-ol system to aid in the separation process design. P-T-x-y equilibrium measurements were obtained for the pentan-2-one + propan-1-ol system at 342.34, 352.05, and 361.65 K and for the pentan-2-one + butan-1-ol system at 342.95, 352.65, and 362.55 K at subatmospheric pressures. The data were successfully modeled using the gamma-Phi approach by employing the Wilson and nonrandom two-liquid activity coefficient models and the Peng and Robinson equation of state for the vapor correction. Thermodynamic consistency testing with the point and area tests was also performed for the experimental VLE data. The data sets passed both the point test with 0.01 tolerance and the area test with 10% tolerance.