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Polymeric electrolyte composites (PECs) based on polymer poly(ethylene oxide) (PEO) and organic clay materials were fabricated. Structural modification and electrochemical properties were investigated for understanding the effects of organic montmorillonite (MMT) in the polymer matrix on the ionic conductivity. For an application to electrolytes of Li batteries, the organic nanoclay fillers were prepared by a cation exchange reaction. XRD results revealed that the interlayer space of organic MMTs were much wider than that of Na⁺-MMT. From the ion conductivity results, PECs containing organic-MMT showed higher conductivity than Na⁺-MMT. This indicated that the improved conductivity is dependent on the reduced crystallinity and enhanced ion-mobility by the increased interlayer spacing of clay fillers.