The gas (O2 and CO2) permeability of an innovative stratified PE–organoclay (LLDPE/OMMT) nano- enabled composite films was studied for the first time and related to the self-assembly process driven by hydrophobic interactions. An 84.4% and a 70% reduction (i.e. a barrier improvement factor of about 6, sufficient for food packaging applications) were observed respectively in the oxygen and carbon dioxide permeability of the 5 bilayers coated film compared to the substrate, while only incorporating 2.4 v/v% of organoclay in the composite and increasing the thickness by 17.7%. Such drastic effect with so low amount of organoclays cannot be achieved by conventional melt blending/exfoliation of the clays into the polymer matrix and is due to a geometrical blocking effect of a brick-wall and compact layer structure of the impermeable clay tactoids. Mathematical prediction of oxygen barrier performance of PE/OMMT films has revealed that 12 bilayers would be necessary to further achieve a barrier improvement factor of 10.

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