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Polymer nanocomposites based on polyphenylene sulfide (PPS) and graphene oxide (GO) modified with cetyltrimethylammonium bromide (CTAB) were prepared. The properties of CTAB-modified graphene oxide (CGO) were investigated by Fourier transform-infrared spectroscopy, X-ray diffraction, and Raman spectroscopy. Results indicated that the ordered structure of GO was impaired by the introduction of CTAB and increased interlayer distance was found for CGO due to the intercalation of CTAB. Mechanical tests revealed that the tensile strength and Young’s modulus of 0.1 wt% CGO/PPS composite were 45.4% and 171.8%, respectively, higher than that of pure PPS matrix, which could be attributed to the entanglement of polymer chains between CTAB and PPS polymer chains. Dynamic mechanical analysis indicated that the glass transition temperature (Tg) of PPS matrix was enhanced due to the addition of CGO and the Tg of 0.5 wt% CGO/PPS composite increased about 10°C higher than pure PPS. In addition, the thermal stability of PPS had significant improvement according to the results of thermogravimetric analysis. The residual mass of 0.5 wt% CGO/PPS composite at 800°C was 1.22 times higher than that of pure PPS.