Advanced electronics demand materials that combine high thermal conductivity with enhanced electrical properties, yet achieving these improvements simultaneously poses significant challenges. This research employs the Taguchi-Grey methodology to explore the synergistic effects of dielectric elements and the high thermal conductivity of epoxy-based composites reinforced with carbon nanotubes (CNTs) and repurposed eggshell particles (ESp). Composite production involved solution blending, followed by evaluations of dielectric constant, thermal conductivity, and sample morphology. Under optimal conditions—1 wt% ESp, 2.5 wt% CNTs, curing at 90 °C for six hours—substantial increases in electrical and thermal conductivity of 19,130% and 94.27%, respectively, were achieved. These enhancements are attributed to the synergistic interaction between dielectric materials and CNTs, as well as the uniform CNT dispersion facilitated by the repurposed eggshells. The 95% confidence level confirmed a strong alignment between the predicted and experimental grey relational grades (GRG), validating the identified optimal parameters. This study demonstrates the potential of using repurposed eggshells to produce conductive polymers with uniformly dispersed CNTs, significantly enhancing thermal conductivity. These findings suggest a promising approach for sustainable, high-performance dielectric materials for electronic applications.