In this study, detailed molecular simulations were used to examine the challenge of selecting metal organic frameworks (MOFs) as filler particles in high performance mixed matrix membranes (MMMs) for separation of H-2 from CH4. The predictions of theoretical permeation models for gas permeability were compared with the experimental data of IRMOE-1/Matrimid, CuBTC/PSF, CuBTC/PDMS and Cu-BPY-HFS/Matrimid MMMs. The good agreement between experiments and our theoretical predictions motivated us to estimate performances of one hundred and nineteen new MOF-based MMMs, composed of seventeen different MOFs and seven different polymers. We identified several MOF-based MMMs exhibiting very high H-2 selectivity and H-2 permeability relative to pure polymer membranes. Finally, we discussed the ways of selecting appropriate MOFs as filler particles for a given polymer matrix which will result in MMMs with promising properties for H-2 separations. (C) 2012 Elsevier B.V. All rights reserved.