Nanocomposite materials with carbon nanotubes and graphene additives have long been considered to be exciting prospective nanomaterials for nanotechnology applications. Some issues of these nanomaterials include poor load transfer, poor interfacial engineering, poor dispersion, and viscosity-related issues, which lead to processing challenges in such nanocomposites, however. Both hydroxylated graphene oxide (GO-OH) and polyketone (PK)-functionalized graphene oxide (GO-PK) were used to improve the properties of polyethylene terephthalate (PET)/PK/graphene oxide (GO) composite fibers. The results showed that there were multiple interactions in the GO-PK. At the molecular level, interactions between PET and PK with GO-PK enhanced their miscibility, and thus, a stable fibril phase structure could be produced following the phase separation. These interactions were demonstrated by various characterization methods. When the fiber with 15 wt % PK/0.1 wt % GO-PK was subjected to 60 min of ultraviolet (UV) treatment, the tensile strength and Young's modulus increased by 37.1 and 77.2% compared with those of 15 wt % PK fibers. This indicated that functionalized graphene oxide has excellent development potential for highperformance nanocomposite fibers.