Diamond/SiC composites offer valuable applications in thermal management because of their exceptional thermal properties. Currently, the predominant method employed for crafting diamond/SiC composites is the reaction sintering approach. However, it encounters the challenge of a high residual silicon content. In this study, we introduced techniques such as bimodal diamond particles and high-density carbon sources (submicron diamond powder) to enhance the diamond content and reduce the residual silicon, optimizing the phase composition. The results indicated the diamond/SiC composite demonstrated a thermal conductivity of 666 W/m·K, a thermal expansion coefficient of 2.73 × 10−6 K−1, and an elastic modulus of 753 GPa. Furthermore, the meticulous assessment of the interface microstructure of diamonds in the diamond/SiC composite was conducted using transmission electron microscopy. The formation of nanocrystal-SiC and interface defects were elucidated by the mechanism of carbon dissolution saturation.