Thin　film　encapsulation　(TFE)　is　one　of　the　key　problems　that　hinders　the　lifetime　and　widespread　commercialization　of　flexible　organic　light-emitting　diodes　(OLEDs).　In　this　work,　TFE　of　OLEDs　with　Al2O3/alucone　laminates　grown　by　atomic　layer　deposition　(ALD)　and　molecular　layer　deposition　(MLD)　as　moisture　barriers　were　demonstrated.　The　barrier　performances　of　Al2O3/alucone　laminates　with　respect　to　the　individual　layer　thickness　and　the　number　of　dyads　were　investigated.　It　was　found　that　alucone　with　suitable　layer　thickness　could　reduce　the　permeation　to　the　defect　zones　of　the　inorganic　layer　by　prolonging　the　permeation　pathway,　sequentially　improving　the　moisture　barrier　performance.　The　water　vapor　transmission　rate　(WVTR)　could　be　further　lowered　with　increasing　the　number　of　dyads　of　the　laminates,　the　WVTR　value　reached　1.44　×　10-4　g　per　m2　per　day　for　laminates　with　5.5　dyads.　These　laminates　were　incorporated　in　OLEDs　with　pixel　define　layer　(PDL),　and　were　found　to　be　able　to　evidently　prolong　the　lifetime　of　the　OLED.　©　2019　The　Royal　Society　of　Chemistry.