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This article presents a review on highly thermostable polymer nanocomposites containing silica, based on author’s own researches, placed in a broader context of the published literature. Thin films based on various polymer matrices, using different alkoxysilanes as precursors of inorganic network, were prepared by sol-gel technique. The influence of silica content and of polymer chemical structure on the thermal, electrical and gas separation properties of the resulting films was investigated. Structure-properties relationships which could be used to design new materials with desired physico-chemical characteristics were established.