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Poly(vinylidene fluoride-co-hexafluoropropylene) (HFP) nanocomposites with layered silicate have been synthesized via the melt extrusion route. The intriguing nanostructure, crystalline structure, morphology, and thermal and mechanical properties of the nanocomposites have been studied and compared critically with pristine polymer. HFP forms intercalated or partially exfoliated nanostructure (or both) in the presence of nanoclay, depending on its concentration. The bombardment of high-energy swift, heavy ions (SHI) on HFP and its nanocomposites has been explored in a wide range of fluence. The nanoclay induces the piezoelectric β-phase in bulk HFP, and the structure remains intact upon SHI irradiation. SHI irradiation degrades pure polymer, but the degradation is suppressed radically in nanocomposites. The heat of fusion of pristine HFP has drastically been reduced upon SHI irradiation, whereas there are relatively minute changes in nanocomposites. The coarsening on the surface and bulk of HFP and its nanocomposite films upon SHI irradiation has been measured quantitatively by using atomic force microscopy. The degradation has been considerably suppressed in nanocomposites through cross-linking of polymer chains, providing a suitable high-energy, radiation-resistant polymeric material. A mechanism for this behavior originating from the swelling test and gel fraction (chemical cross-linking) as a result of SHI irradiation has been illustrated. [ABSTRACT FROM AUTHOR]