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Composites of poly(vinyl alcohol) (PVA) with sulfonated graphene (SG) show fibrillar, dendritic and rod like structures for SG1, SG3 and SG5 samples, respectively, where the number indicates weight percent of SG. Differential scanning calorimetry shows a new peak in addition to that of PVA arising from the supramolecular organization of the components in SG1 and SG3. Seventeen percent and 36% increases of PVA crystalline thickness and 77% and 79% increases in amorphous overlayer thickness for SG1 and SG3 over PVA are evident from small angle X-ray scattering results but SG5 does not show any change. Atomic force microscopy results of SG suggest aggregation at higher concentration and the composites exhibit composition dependent mechanical properties with the highest increase of stress (177%), strain at break (45%) and toughness (657%) in SG3 over PVA. Young’s modulus increases with …