Tungsten- and nickel-containing coatings have been produced on the surface of synthetic diamond crystals by rotary chemical vapor deposition (RCVD) using tungsten hexacarbonyl, W(CO)6, and nickelocene, Ni(C5H5)2, as gaseous precursors. The thickness, composition, and morphology of the coatings have been shown to depend on the RCVD process duration and reactant concentrations in the vapor phase. The synthetic diamond microcrystals with tungsten- and nickel-containing coatings have been used to produce copper–diamond heat-conducting composites. Powder mixtures containing 50 vol % diamond with a particle size of 50, 100, or 200 μm have been consolidated by spark plasma sintering or hot pressing. It has been shown that the highest relative density (97%) and thermal conductivity (340 W/(m K)) are offered by the composites produced by spark plasma sintering using tungsten carbide-coated 50-μm diamond crystals.