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In this study, surfaces of copper plates were coated with a thick alumina layer by the plasma spray coating to fabricate a composite with a dielectric performance that made them suitable as substrates in electronic devices with high thermal dissipation. The performance of alumina dielectric layer fabricated by the plasma spray coating and traditional screen-printing process was compared, respectively. Effects of the spraying parameters and size of alumina particles on the microstructure, thickness, and the surface roughness of the coated layer were explored. In addition, the thermal resistance perpendicular to the interface of copper and alumina and the breakdown voltage across the alumina layer of the composite were also investigated. Experimental results indicated that alumina particles with 5-22 μm in diameter tended to form a thicker layer with a poorer surface roughness than that of the particles with 22-45 μm in diameter. The thermal resistance increased with the surface roughness of the alumina layer, and the breakdown voltage was affected by the ambient moisture, the microstructure and the thickness of the layer. The optimal parameters for plasma spray coating were an alumina powder of particles size between 22 and 45 μm, a plasma power of 40 kW, a spraying velocity of 750 m/s, an argon flow rate of 45 L/min, a spraying distance of 140 mm, and a spraying angle of 90°. It can be concluded that an alumina layer thickness of 20 μm provided a low surface roughness, low thermal resistance, and highly reliable breakdown voltage (38 V/μm).