Two trimellitic anhydride-functionalized, thermally reduced graphenes with different aspect ratios, A f, and the same C/O ratio (8:1) were prepared and melt-mixed into poly­(ethylene terephthalate) (PET), and the mechanical properties of the resulting nanocomposites were studied with a focus on plastic deformation behavior. A slight increase in the G′ of the melt was observed for the surface-modified low-A f graphene composites (A f = 20) below the percolation threshold, whereas a significant enhancement in G′ was observed for higher-A f graphene composites (A f = 80) at all graphene loadings, both below and above the percolation concentration. Furthermore, the use of modified low-A f graphene caused an improvement both in Young’s modulus and elongation at break of the resulting PET nanocomposites because of enhancement of interfacial adhesion between filler and matrix which resulted in the formation of a coupled network via covalent bonding and the suppression both of strain-induced orientation and strain-induced crystallization. By contrast, the use of modified higher-A f surface graphene in nanocomposites caused a drastic improvement in Young’s modulus but lower elongation-at-break than with the unmodified counterpart; the former effect is due to the formation of denser coupled networks and stronger interfacial adhesion as a result of graphene surface modification and the latter is due to the added geometrical restriction in unentangling chains from the PET matrix in the presence of higher-A f graphene. The preceding observations demonstrate the potential impacts of tuning both surface chemistry and aspect ratio of graphene in the fabrication of PET/graphene composites.