Ti3SiC2, a ternary carbide, was proposed at this paper to use as the binder of polycrystalline diamonds to overcome the weaknesses of traditional metal binders and ceramic binders. Ti3SiC2was first reported to be in-situ synthesized under high pressure (4GPa) and at high temperature (1400°C) (HPHT) from the mixtures of Ti, Si and graphite powders or the mixture of Ti, SiC and graphite powders. Ti3SiC2-damond composites were also made at HPHT from the previous mixtures and diamond particles. TiCx, Ti5Si3Cxand TiSi2were main impurities and/or intermediate products of Ti3SiC2samples synthesized at HPHT. Ti3SiC2content increased as synthesized time increased from 10 min to 60 min. For as-synthesized composites, diamond particles were evenly distributed in matrix. The diamond particles are bonded well with the matrix by three types of interface.