Vapor-liquid equilibria (VLE) of the binary mixtures nitrogen + acetone and oxygen + acetone are studied by molecular simulation and experiment. A force field model for pure acetone (CH3-(C=O)-CH3) is developed, validated, and then compared with four molecular models from the literature. The unlike dispersive interaction between nitrogen and acetone as well as oxygen and acetone is adjusted. On the basis of these mixture models, the VLE of nitrogen + acetone and oxygen + acetone is determined by molecular simulation and validated on the basis of experimental data. To extend the experimental database, a gas solubility apparatus is constructed and the saturated liquid line of nitrogen + acetone is measured at the three isotherms 400 K, 450 K, and 480 K up to a maximum pressure of 41 MPa. Finally, the results from simulation and experiment are used to parametrize the Peng-Robinson EOS for nitrogen + acetone with the Huron-Vidal mixing rule.