In this paper, new experimental vapour-liquid equilibrium data of the furan + n-hexane and furan + toluene binary systems are reported. The data are determined using the ebulliometric technique. The measured data are used to assess the predictions obtained with molecular simulation, a group contribution polar PC-SAFT model and the COSMO-RS and COSMO-SAC approaches. For this purpose, new force field parameters (needed in MC-simulation) are determined for furans by fitting a limited amount of saturation data. In GC-PPC-SAFT, most of the parameters were adopted from previous studies with exception of the polar moments (dipoles are taken from experimental data). The mixtures phase diagrams are predicted (without binary parameters) at atmospheric pressure using these newly determined parameters as well as those of hexane and toluene determined in earlier studies.The predicted results are consistent with the new experimental data. Nevertheless, for the furan + n-hexane binary system, it appears that a binary interaction parameter is necessary to correctly correlate the data and to satisfactory describe the literature excess enthalpy data.