Developing　catalysts　for　the　selective　oxidation　of　alkenes　with　environment-friendly,　unique　structural　characteristics,　high　economic　benefit　and　better　catalytic　performance　is　important.　Herein,　we　employed　ZIF-67　as　the　sacrificial　template　to　synthesize　bimetallic-organic　frameworks　CoxMo100-x-ZIF　nanocages　by　a　facile　dissolution-regrowth　strategy.　The　Co51.8Mo48.2-ZIF　catalyst　was　tested　under　various　experimental　parameters　for　the　selective　oxidation　of　cyclooctene　to　screen　the　optimal　reaction　conditions.　Under　the　optimal　reaction　conditions,　Co51.8Mo48.2-ZIF　nanocages　exhibited　a　high　cyclooctene　conversion　of　99.3　%　and　a　selectivity　of　99.0　%　to　epoxy　cyclooctane.　Furthermore,　Co51.8Mo48.2-ZIF　nanocages　can　maintain　their　catalytic　performance　after　reused　five　catalytic　cycles.　This　bimetallic　catalyst　could　also　be　used　for　the　epoxidation　of　a　wide　range　of　alkenes,　such　as　hexene　or　cyclohexene.　In　addition,　the　kinetic　studies　were　conducted,　and　a　reasonable　reaction　mechanism　was　proposed　based　on　density　functional　theory　calculations.　The　outstanding　catalytic　performance　of　CoxMo100-x-ZIF　nanocages　can　be　attributed　to　the　cooperativity　between　Co　and　Mo　sites　and　the　hollow　structure　with　high　surface　areas.　©　2020　Wiley-VCH　GmbH