Abstract: Solvent diffusion phenomenon in polymeric materials widely exists in both daily life and industrial processes,thus it is of universal significance to study on it.Vrentas and Duda proposed a model based on the free-volume theory to predict diffusion coefficients of low molecular weight solvent in polymeric materials.All parameters in the model were determined by solvent and polymer molecule properties respectively, without any direct diffusivity measurement.Using the Vrentas-Duda model, solvent diffusion coefficients in typical polymer/solvent systems were predicted and compared with experimental data for evaluating availability of the model. For most amorphous rubbery polymeric material systems,the Vrentas-Duda model gave satisfying accuracy for calculating solvent diffusion coefficients, except for the complicated systems with hydrogen bond. This calculation also showed better accuracy for solvent self-diffusion coefficients than mutual-diffusion coefficients.