Large　defects　have　important　impact　on　performance　of　separation　membranes.　In　this　paper,　in　order　to　reduce　the　large　defects　of　the　industrial　ceramic　supports,　we　prepared　a　nanohybrid　separation　membrane　with　a　selective　layer　and　a　sub　layer　on　the　macroporous　substrate　with　polyelectrolyte-coated　nanoparticles.　SEM,　EDS　and　pore　size　analyses　suggest　that　the　although　ZrO2　nanoparticles　can　migrate　into　the　large　defects　to　modify　the　membrane　pores,　the　matching　of　pore-mouth　size　and　diameter　of　NPs　plays　important　role　in　the　in　situ　modification　of　the　substrates.　The　integrality　of　the　as-prepared　nanohybrid　multilayer　membrane　was　evaluated　in　the　nanofiltration　of　dye　solutions.　The　organic-inorganic　composite　membranes　perform　high　flux　and　retention　for　separation.　Membranes　were　prepared　to　study　the　separation　performance　on　different　substrates　and　with　different　building　blocks　(polyelectrolyte　molecule　weights　and　polyelectrolyte　molecule　structure).　We　found　that　the　pore-mouth　size　of　substrates　and　the　structure　of　building　blocks　mainly　affected　the　structure　and　the　nanofiltration　performance　of　the　composite　membranes.　Such　assembly　allow　us　to　in　situ　modify　the　large　defects　of　inorganic　substrates　while　preparing　the　selective　layer.　(C)　2017　Elsevier　B.V.　All　rights　reserved.