Oxidative　dehydrogenation　of　propane　with　carbon　dioxide　(CO2-ODP)　characterizes　the　tandem　dehydrogenation　of　propane　to　propylene　with　the　reduction　of　the　greenhouse　gas　of　CO2　to　valuable　CO.　However,　the　existing　catalyst　is　limited　due　to　the　poor　activity　and　stability,　which　hinders　its　industrialization.　Herein,　we　design　the　finned　Zn-MFI　zeolite　encapsulated　noble　metal　nanoparticles　(NPs)　as　bifunctional　catalysts　(NPs@Zn-MFI)　for　CO2-ODP.　Characterization　results　reveal　that　the　Zn2+　species　are　coordinated　with　the　MFI　zeolite　matrix　as　isolated　cations　and　the　NPs　of　Pt,　Rh,　or　RhPt　are　highly　dispersed　in　the　zeolite　crystals.　The　isolated　Zn2+　cations　are　very　effective　for　activating　the　propane　and　the　small　NPs　are　favorable　for　activating　the　CO2,　which　synergistically　promote　the　selective　transformation　of　propane　and　CO2　to　propylene　and　CO.　As　a　result,　the　optimal　0.25%Rh0.50%Pt@Zn-MFI　catalyst　shows　the　best　propylene　yield,　satisfactory　CO2　conversion,　and　long-term　stability.　Moreover,　considering　the　tunable　synergetic　effects　between　the　isolated　cations　and　NPs,　the　developed　approach　offers　a　general　guideline　to　design　more　efficient　CO2-ODP　catalysts,　which　is　validated　by　the　improved　performance　of　the　bifunctional　catalysts　via　simply　substituting　Sn4+　cations　for　Zn2+　cations　in　the　MFI　zeolite　matrix.　©　2023　Science　Press　and　Dalian　Institute　of　Chemical　Physics,　Chinese　Academy　of　Sciences