Ethylene　production　from　oxidative　coupling　of　methane　is　a　sustainable　and　economically　attractive　alternative　to　that　through　traditional　hydrocarbon　cracking　technology.　However,　efficient　ethylene　separation　from　the　complex　reaction　mixture　is　a　daunting　challenge　that　hinders　the　practical　adoption　of　this　technology.　Herein,　we　report　the　efficient　adsorptive　separation　of　the　CH4/CO2/C2H4/C2H6　mixture　using　three　representative　metal-organic　frameworks　(MOFs)　(UTSA-74,　MOF-74,　and　HKUST-1)　with　diverse　open　metal　sites.　The　efficient　separation　relies　on　tuning　the　selectivity　through　the　convergence　of　characteristics　including　Lewis　acidity　of　open　metal　sites,　pore　space,　and　cooperative　binding　behavior.　The　separation　performance　of　these　materials　has　been　evaluated　through　single-component　gas　adsorption　and　dynamic　breakthrough　experiments.　HKUST-1　provides　the　highest　separation　potential　(4.1　mmol/g)　thanks　to　its　simultaneously　high　ideal　adsorbed　solution　theory　(IAST)　selectivity　and　ethylene　adsorption　capacity,　representing　a　benchmark　material　for　such　a　challenging　quaternary　separation.