Isobaric vapor liquid equilibrium (VLE) data for the binary mixture of glycerol ethyl acetal (GEA) and acetonitrile were measured at 60.0 kPa and 97.8 kPa, using a dynamic recirculating still. The VLE data were correlated using the nonrandom two-liquid (NRTL) and universal quasichemical activity coefficient (UNIQUAC) models, and the interaction parameters of this mixture were estimated. The experimental procedure was checked by measuring VLE data at 97.8 kPa of the well-known system acetone/methanol showing high conformity, as given by applying a set of VLE consistency tests. The vapor pressure of GEA was measured, for the first time, in the temperature range from 371.85 K to 456.85 K, and it is described by the following expression: In P-GEA(SAT)(Pa) = 24.17 - 5781/T(K). The information collected is of utmost importance for the purification of GEA synthesized using simulated moving bed reactor technology.