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Summary: High‐density polyethylene (HDPE) micro‐ and nanocomposites with spherical and platelike inclusions were prepared and the effect of filler particles on polymer crystallinity and gas permeability was investigated. Platelike inclusions strongly reduce the polymer permeability coefficient, while spherical ones have no influence on it, irrespective of their size. The reduction in gas permeability depends on the average aspect ratio of the inclusions, which in turn depends on the exfoliation of the organo‐montmorillonites (OM) and consequently on its surface treatment.A TEM micrograph of 3 vol.‐% 2C18 · M‐HDPE nanocomposite, showing partial exfoliation of the organo‐montmorillonite.imageA TEM micrograph of 3 vol.‐% 2C18 · M‐HDPE nanocomposite, showing partial exfoliation of the organo‐montmorillonite.