Good interfacial adhesion is typically correlated to obtaining the best tensile/flexural performance for carbon fibre-reinforced composites. The nature or even presence of the interphase, a localized region around the fibre-matrix junction, is often discussed but notoriously difficult to visualize and characterise. Here, a surface-initiated electro-polymerization approach to covalently graft either polyacrylamide or polygylcidyl methacrylate to the carbon fibres was used. This was followed by continuous melt compounding into the polyamide-6 matrix prior to injection moulding. Analysis via X-ray photoelectron spectroscopy (XPS) coupled with topological/visual study through scanning electron microscopy (SEM), showed distinct surface changes after modification and at the composite fracture surface. Additionally, mechanical (tensile, flexural, and tribological characteristics) and thermal (differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA)) investigations were performed. The results showed that the unmodified CF samples exhibit higher tensile and flexural modulus than the modified CF samples. However, the wear rate has been significantly decreased for modified CF samples. SEM of fractured composite surfaces showcased a clear interphase region surrounding the fibre, highlighting the importance of interphase/interphase mechanics in the design of optimal composite interfaces.