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The preparation of graphene (GN) and graphene-intercalated halloysite nanotubes (HNTs) to form nanomaterials was achieved by using HNTs template. As a promising application, a series of the polytetrafluoroethylene (PTFE) nanocomposite filled with GN and GN/HNTs at different mass fractions were prepared. The mechanical and friction properties of PTFE nanocomposites depending on the mass fraction of graphene-intercalated HNTs (GN/HNTs) were intensively investigated. The comparison between the effects of GN and GN/HNTs serving as fillers on properties of PTFE was presented. The results showed that in terms of enhancing the tensile strength of PTFE, the enhancement effect of GN is superior to GN/HNTs, and in terms of the elongation at break, the GN/HNTs filler could reserve more toughness than GN. The Young’s modulus of the GN/HNTs incorporated into PTFE is about 1.9 times larger than pure PTFE, and is superior to GN/HNTs. The friction coefficient of PTFE nanocomposites filled with GN and GN/HNTs was slightly higher than pure PTFE and the latter was lower than the former. The volume wear rate of PTFE nanocomposites filled with GN/HNTs was obviously lower than the case with GN, which exhibited the better wear resistance of GN/HNTs used as filler