Thin　film　encapsulation　(TFE)　with　high　barrier　performance　and　mechanical　reliability　is　essential　and　challenging　for　flexible　organic　light-emitting　diodes　(OLEDs).　In　this　work,　SF6　plasma　treatments　were　introduced　for　surface　modifications　of　acrylic　in　Al2O3/acrylic　laminates　fabricated　by　atomic　layer　deposition　(ALD)　and　ink-jet　printing　(IJP).　It　was　found　that　micro-/nano-structures　and　surface　fluoridation　appeared　on　the　surface　of　acrylic,　and　could　be　modulated　by　the　discharge　power　and　irradiation　of　plasma　treatment.　The　water　vapor　transmission　rates　(WVTR)　of　Al2O3/acrylic　multi-layers　decreased　evidently　because　of　reducing　surface　polarity　and　strong　cross-link　of　acrylic　after　plasma　treatments.　Furthermore,　the　rugged　surface　and　relieved　residual　stress　resulted　from　etching　and　heating　of　acrylic　could　enhance　the　mechanical　property　remarkably.　The　plasma　treated　Al2O3/acrylic　multi-layers　with　only　3　dyads　exhibited　a　low　WVTR　value　of　1.02　×　10−6　g/m2/day　and　more　stable　mechanical　property　under　200　iterations　blending　test　by　comparative　measurements,　proving　that　the　introduction　of　SF6　plasma　surface　modifications　could　improve　simultaneously　the　barrier　performance　and　mechanical　reliability　prominently　of　the　inorganic/organic　multi-layers　with　no　need　of　extra　neutral　axis　design.　©　2021　Elsevier　B.V.