Usually olefin/paraffin separations (e.g., ethane/ethylene and propane/ propylene) by distillation process are energy-intensive because such molecules have very similar molecular size and boiling point. Membrane process has been considered as an alternative method to achieve energy- efficient olefin/paraffin separation. However, based on solution-diffusion mechanism, it is hard to design good membrane materials to separate them efficiently. Here we report fundamental separation properties of olefin/paraffin through graphene oxide (GO) membranes having slit-like channels. Analogue to carbon molecular sieve membranes, GO membranes showed ability to separate these molecules. To improve the separation properties, GO membranes have been modified by various methods.