Molecular　sieve-based　membranes　are　considered　to　be　promising　for　achieving　both　high　selectivity　and　permeability.　Layered　double　hydroxides　(LDHs)　are　typical　two-dimensional　crystalline　compounds　with　highly　uniform　interlayer　galleries　that　can　be　used　to　construct　efficient　molecular　transport　pathways.　Herein,　vertically　channeled　laminates　are　constructed　on　a　tubular　alumina　substrate　using　CoAl-LDH　as　building　blocks.　Good-quality　laminates　are　crystallized　by　direct　nucleation　and　growth　onto　the　alumina,　in　which　alumina　substrates　act　as　both　reactants　and　supports.　Vertically　aligned　interlayer　galleries　are　formed　as　sieving　and　transport　channels　for　water　molecules　with　the　oriented　nucleation　effect　of　NH4F.　Compared　with　the　zigzag　pathways　formed　by　two　dimensional　materials　parallel　to　the　substrate,　the　straight　vertical　channels　have　higher　molecular　transfer　efficiency.　As　a　result,　the　robust　CoAl-LDH　membranes　show　much　higher　and　more　stable　organic　solvent　dehydration　performance　than　most　membranes　under　a　wide　range　of　feed　conditions.　This　work　thus　demonstrates　that　LDH-based　composite　membranes　are　highly　promising　as　the　next　generation　of　membranes　for　molecular　sieving.