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Iron/polytetrafluoroethylene (Fe/PrFE) nanocomposites were prepared by means of high-energy ball milling for different lengths of time. Three new components of FeF2, FeF3, and Fe3C in the resultants were mainly investigated using the M(o)ssbauer spectroscopy (MS). The components and average grain size of the nanocomposites were also measured using X-ray diffraction (XRD) and transmission electron microscopy (TEM), respectively.