Colloidal　metal-organic　framework　(MOF)　nanoparticles,　with　tailored　asymmetric　nanoarchitectures　and　hierarchical　meso-/microporosities,　have　significant　implications　in　high-performance　nanocatalysts,　nanoencapsulation　carriers,　and　intricate　assembly　architectures.　However,　the　methodology　that　could　achieve　precise　control　over　the　anisotropic　growth　of　asymmetric　MOF　particles　with　tailored　distributions　of　meso-　and　microporous　regions　has　not　yet　been　established.　In　this　study,　we　introduce　a　facile　anisotropic　interface　successive　assembly　approach　to　synthesize　asymmetric　core-shell　MOF　(ZIF-67)　nanobowls　with　worm-like　mesopores　in　the　core　and　intrinsic　micropores　in　the　shell.　Our　synthesis　pathway　relies　on　anisotropic　nucleation　of　mesoporous　MOF　nanohemispheres　on　emulsion　interfaces　through　the　cooperative　assembly　of　surfactants　and　MOF　precursors.　This　is　followed　by　the　growth　of　microporous　MOF　layers　on　both　interfaces　of　mesoporous　cores　and　emulsion　droplets,　resulting　in　a　hierarchically　porous　core-shell　nanostructure.　By　utilizing　this　multi-interface-driven　approach,　we　enable　the　creation　of　diverse　geometries　and　distributions　of　mesopores　and　micropores　in　asymmetric　MOF　nanoarchitectures.　The　obtained　bowl-like　meso-/microporous　core-shell　ZIF-67　particles　exhibit　enhanced　catalytic　activity　for　CO2　cycloaddition,　attributed　to　reactant　accumulation　within　the　bowl-like　architecture,　active　site　accessibility　in　the　open　mesoporous　core,　and　improved　structural　stability.　Overall,　our　study　provides　insights　and　inspiration　for　exploring　the　intricate　asymmetric　nanostructures　of　hierarchically　porous　MOFs　with　diverse　potential　applications.　©　2023　American　Chemical　Society.