A fast, noninvasive, and efficient analytical measurement strategy for the characterization of vapor-liquid equilibria (VLE) is presented, which is based on phase (state of matter) selective Raman spectroscopy in multiphase flows inside microcapillay systems (MCS). Isothermal VLE data were measured in binary and ternary mixtures composed of acetone, water, carbon dioxide or nitrogen at elevated pressures up to 10 MPa and temperatures up to 333 K. For validation, the obtained data were compared with literature data and reference measurements in a high-pressure variable volume cell. Additionally, the mixtures were investigated at temperatures and pressures where no data is available in literature to extend the high-pressure VLE database.