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Novel composite carbon particles are developed that can self-assemble as a coating on a substrate without a binder. These carbon particles were used as a coating to enhance thermal dissipation and their thermal conductivity, surface emissivity and cooling performance were measured. Carbon particles with both thiol and epoxy functional groups self-assembled to form a coating on the surface of a heat sink without a binder, which greatly improved the thermal conductivity of the coating. Coating a heat sink with the carbon particles yielded a higher thermal conductivity and emissivity than could be obtained with the addition of binder in the conventional approach, and significantly enhanced the cooling performance. In addition, the cooling performance of the carbon nanotube outperformed all other particles when coated on a substrate, because it had the highest thermal conductivity and good radiation emissivity. We developed an equation to describe the various parameters affecting the cooling performance of the thermally dissipative coating. This equation was confirmed by the experimental data.