With increased focus on miniature high power density electronic packages, there is a need for the development of new interface materials with lower thermal resistance. To this end, high conductivity thermal paste or similar thermal interface materials (TIMs), reinforced with superior thermal conductivity materials such as multi-walled carbon nanotubes (MWCNTs), graphene nanoplatelets (GNPs), graphite-derived multilayer graphene (g-MLG) offer an effective strategy to provide efficient paths for heat dissipation from heat source to heat sink. In an earlier paper, we had demonstrated that multilayer graphene derived from coal (coal-MLG) synthesized using our in-house developed one-pot process, has increased presence of phenolic groups on its surfaces, which translates into better dispersion of coal-MLG in silicone thermal paste. In this paper, we first compare the thermal conductance of a high conductivity thermal paste (k = 8.9 W/mK) using coal-MLG as an additive with that realized with other nano additives — MWCNTs, GNPs, and g-MLG. The data shows that coal-MLG as an additive outperforms all the other investigated nano additives in enhancing the thermal performance of the paste. With the coal-MLG as an additive, ∼70% increase in thermal performance was observed as compared to the base thermal paste used. This increase is about 2.5 times higher than that obtained using g-MLG as an additive. We also measured the thermal performance of coal-MLG-based TIM with its different wt.% fractions. The data confirmed our hypothesis that the optimum level of the loading fraction of the additive that can be dispersed in the matrix (paste in this case) before the onset of agglomeration is higher for the coal-MLG (3%) than for the other additives (2%). The implication is further improvement thermal performance with coal-MLG. The data shows the additional thermal enhancement to ∼2X. Finally, since coal-MLG produced by our in-house process is relatively cheaper and more environmentally friendly, we believe that these results would pave the path for enhanced thermal performance with non-silicone thermal pastes at a significantly lower cost. We also expect similar benefits for the silicone-based thermal pastes.