Isobaric vapor-liquid equilibrium (VLE) data for the systems of 3-methylthiophene with four compounds (2,3-dimethyl-2-butene, n-heptane, toluene and 2-methylbutane) were measured at 101.33 kPa with a modified Rose-Williams still. Gas chromatography was used to analyze compositions of the samples from the vapor-liquid equilibrium systems. All the VLE measurements passed the thermodynamic consistency test proposed by Herington and showed positive deviations from Raoult's law. The experimental data of binary systems were correlated by Wilson model for the liquid phase and also compared with original UNIFAC and UNIFAC-Dortmund predictive models. Results showed that the original UNIFAC model gave better predictions than the UNIFAC-Dortmund model. (C) 2012 Elsevier B.V. All rights reserved.