This research investigates a novel hybrid E-glass fiber coated with a thin amorphous carbon (coke) layer, referred to as GF@C, designed to enhance the affinity of fiber with a polymer matrix. Acrylonitrile butadiene styrene (ABS), an engineering thermoplastic, was selected as the matrix to form the composite. The carbon coating was produced by pyrolyzing a lubricant oil (Lo) layer applied to the glass fiber strands. To promote the formation of graphite crystallites during carbonization, a small amount (x wt.% of Lo) of coronene (Cor) was added to Lo as a dopant. The resulting doped fibers, denoted GF@C_Lo-Cor(x%), were embedded in ABS at 70 wt.%, leading to significant improvements in mechanical properties. At the optimal doping level (x = 5), the composite achieved a Young’s modulus of 1.02 GPa and a tensile strength of 6.96 MPa, substantially higher than the 0.4 GPa and 3.81 MPa observed for the composite with the pristine GF. This enhancement is attributed to a distribution of graphite crystallites and their graphitization extent in the carbon coating, which improves interfacial bonding and increases chain entanglement. Additionally, GF@C_Lo-Cor(x%)–ABS composites (x = 0 and 5) exhibit significantly higher dielectric constant–temperature profiles than GF–ABS, attributed to the formation of diverse chain adsorption states on the C-coating.