Metal organic frameworks (MOFs) have been widely studied as adsorbents and membranes for gas separation applications. Considering the large number of available MOFs, it is not possible to fabricate and test the gas separation performance of every single MOF using purely experimental methods. In this study, we used molecular simulations to assess both adsorption-based and membrane-based CH4/N-2 separation performances of 102 different MOFs. This is the largest number of MOF adsorbents and membranes studied to date for separation of CH4/N-2 mixtures. Several adsorbent evaluation metrics such as adsorption selectivity, working capacity, and regenerability were predicted, and the top performing adsorbents were identified. Several MOFs were predicted to exhibit higher adsorption selectivities than the traditional adsorbents such as zeolites and activated carbons. Relation between adsorption-based separation performances of MOFs and their structural properties were also investigated. Results showed that MOFs having the largest cavity diameters in the range of 4.6-5.4 angstrom, pore limiting diameters in the range of 2.4-3.7 angstrom, surface areas less than 2000 m(2)/g, and porosities less than 0.5 are promising adsorbents for CH4/N-2 separations. We then combined adsorption and diffusion data obtained from molecular simulations and predicted both membrane selectivities and gas permeabilities of MOFs for separation of CH4/N-2 mixtures. A significant number of MOF membranes were identified to be CH4 selective in contrast to the traditional membrane materials which are generally N-2 selective. Several MOFs exceeded the upper bound established for the polymeric membranes, and many MOFs exhibited higher gas permeabilities than zeolites. The results of this study will be useful to guide the experiments to the most promising MOF adsorbents and membranes for efficient separation of CH4/N-2 mixtures.