The　bimetallic　ion　exchanged　clinoptilolites　(M1xM2y-CPs,　M1　=　Li+,　Na+　or　Cs+,　M2　=　Li+　or　Cs+,　x,　and　y　=　the　exchange　degree　of　the　first　and　second　cation)　were　prepared.　Their　physic-chemical　parameters　were　characterized　using　various　methods.　The　results　demonstrated　that　the　relative　crystallinity　of　M1xM2y-CPs　gradually　decreased　with　the　increase　of　the　secondary　cationic　introduction.　Meanwhile,　M1xM2y-CPs　presented　the　surface　fractal　features,　particularly,　the　values　of　M1xM2y-CPs　were　higher　than　that　of　single　ion　exchanged　CPs,　suggesting　that　the　surface　of　M1xM2y-CPs　was　rougher　and　more　disordered.　The　effects　of　the　type,　size,　and　distributions　of　the　used　various　cations　on　the　gas　adsorption　and　separation　properties　were　evaluated　via　their　equilibrium　adsorbed　performances　of　CO2　and　CH4　demonstrate.　The　results　indicated　that　the　CO2　uptake　of　NaxLiy-CP　increased　with　the　increase　of　Li+　exchange　degree,　in　which,　Na67.95Li17.15-CP　presented　the　maximum　adsorption　capacity　of　2.45　mmol/g　for　CO2.　While,　the　CO2/CH4　selective　factors　of　NaxCsy-CP　were　around　10.82-12.75　at　273　K　and　9.92-12.44　at　298　K,　much　higher　than　that　of　other　bimetallic　ion　exchanged　samples.　The　breakthrough　experiments　displayed　a　longer　breakthrough　time　and　a　stronger　CO2　absorption　capacity.　The　cycling　tests　indicated　an　excellent　CO2　adsorption　stability　and　reversibility.　Furthermore,　the　kinetics　adsorption　of　pseudo-first-order　and　intraparticle　model　were　used　to　investigate　their　adsorption　mechanism.　Finally,　the　CO2　adsorption　mechanism　between　the　adsorption　amount　and　the　average　total　energy　of　the　CO2　adsorption　system　was　preliminary　elucidated　using　Material　Studio　simulation　software.