Under the condition of 5.6 GPa and 1250–1450 ℃, the diamond single crystals are synthesized in a cubic anvil high-pressure and high-temperature apparatus. High-purity FeNiCo solvents or NiMnCo solvents are chosen as the catalysts. High-purity (99.99%) graphite powders selected as a carbon source. High-quality abrasive grade diamond single crystals with relatively developed (100) or (111) crystal planes are used as crystal seeds. The effects of catalyst composition on crack defects in diamond single crystals are studied carefully. Firstly, using FeNiCo and NiMnCo catalysts respectively, we carry out the diamond single crystal growth experiments. It is found that under the same crystal growth condition, the probability of crystal crack defects in diamond single crystals grown with FeNiCo catalyst is significantly higher than that of crystals grown with NiMnCo catalyst. We believe that this is related to the high viscosity, poor fluidity of FeNiCo catalyst melt, and the large specific surface area of the crystal during growth, which leads to its high requirements for the stability of growth conditions. Secondly, the relationship between the growth time and the limit weight gain speed of the diamond single crystal synthesized, respectively, by FeNiCo catalyst and NiMnCo catalyst are investigated. The results are shown below. 1) The limiting growth rate of diamond single crystal increases with the growth time going by. 2) In the same growth time, the limit growth rate of diamond crystal grown with NiMnCo catalyst is higher than that of diamond crystal grown with NiMnCo catalyst. Thirdly, by scanning electron microscopy (SEM), we calibrate the surface morphology of the synthesized diamond single crystal. The test results show that the diamond single crystal has a high surface flatness. Even for the crystals with crack defects in the interior, the surface flatness is still good. However, Fourier transform infrared (FTIR) measurements show that the nitrogen impurity content of diamond crystal grown by FeNiCo catalyst with crack defect is about 3.66×10 ^–4. The content of nitrogen impurity in the crystal grown by NiMnCo catalyst without crack defect is about 4.88×10 ^–4. The results show that there is no direct correlation between nitrogen impurity content and crack defects in diamond crystal.