Exfoliated　montmorillonite　(MMT)　nanosheets　were　aligned　and　self-assembled　with　poly(vinyl　alcohol)　(PVA)　to　form　highly　ordered　laminate　nanocoatings　on　the　surface　of　polymeric　thin　films　to　impart　excellent　barrier　properties　as　well　as　dielectric　enhancement.　In　this　paper,　the　dielectric　properties　of　polymer　thin　films　with　nanoclay　coatings　were　investigated.　A　remarkable　improvement　in　the　breakdown　strength　of　LDPE　and　Kapton　(R)　films　with　the　application　of　nanoclay　coating　was　discovered.　In　addition,　the　dielectric　spectroscopy　study　of　BOPP　and　Kapton　r　films　indicated　a　much　improved　thermal　stability　in　their　permittivity　response　with　the　application　of　the　nanoclay　coatings.　Such　improvement　in　the　thermal　stability　of　dielectric　response　was　achieved　without　obvious　increase　of　the　dielectric　dissipation　factors.