By temperature gradient method (TGM), with Invar alloy as solvent catalyst, FeS and boron as additives, large diamond crystals are grown under high pressure and high temperature (HPHT) of about 5.4GPa and 1550K. With the content of FeS increased, the colors of grown crystals would be changed from transparent yellow to opaque gray-black, and the quality of diamond crystals could also be destroyed markedly. When both boron and FeS co-doped, the negative effect of FeS on crystal quality could be eliminated somewhat. To a certain content of FeS, with the boron content increased, the crystal color would be changed from opaque gray-black to transparent yellow, and boron content needed is related directly to FeS content in growth systems. The nitrogen content in diamond lattice decreases greatly, with FeS content increased in the growth system, and a 1050cm-1 absorption peak in IR spectrum is also present in diamond crystals grown in FeNi-FeS-C system.