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Metal/diamond composites have been considered as the new generation of thermal management material. The critical challenge to obtain composites with high thermal conductivity (TC) is to improve the interfacial bonding between the matrix and diamond. In the present study, a titanium coating was plated on the surface of diamond particles via vacuum evaporation–deposition, and Al/diamond composites were consolidated by spark plasma sintering (SPS) technique. The TC and microstructure of composites, respectively, with coated and uncoated diamond particles are compared and discussed. The results show that the Ti coating can significantly increase the wetting property between Al and diamond, leading to a strong interfacial bonding. The diffusion of Ti into the matrix and the formation of TiC are detected at the Al–diamond interface. The properties of composites, respectively, with coated and uncoated diamond exhibit different trends with increasing sintering temperature or diamond volume fraction. Compared with composites with uncoated particles, the Al/Ti–diamond composites obtained the much higher relative density and TC as high as 491 W/mK. Based on the comparison between the experimental and theoretical values, it is found that the thermal conductivities of Al/Ti–diamond composites have reached or surpassed the theoretical calculations with the particle volume fraction not more than 50%. [ABSTRACT FROM AUTHOR]