In this work, diamond crystals were synthesized with N–H–O impurities by the temperature gradient method (TGM) under high pressure and high temperature (HPHT) conditions using FeNi alloy as the metal solvent (MS). The results indicated that the spontaneous nucleation rate and proportion, growth characteristics, surface growth texture, and the impurity concentration of diamond crystals changed drastically upon changing the impurity content in the system. Mutual diffusion between the MS and carbon source (CS) was also blocked, which seriously inhibited the growth rate of diamond crystals. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses corroborated that the zero-valent iron (Fe0) and nickel (Ni0) contents declined after N–H–O impurities were introduced. The newly formed graphite can be found in the MS, but the ferric carbide disappears. XPS also confirmed shifts in the binding energy of FeNi MS peaks, more iron oxide and nickel oxide were identified in MS, hindering the mass transfer process. CO and NO were absorbed on the surface of MS, which hindered the surface processes of diamond growth. The formation of intermediates (Fe3C) was impeded during diamond growth and blocked the spontaneous nucleation of diamond. All of these phenomena contributed to a poor growth rate and changed the surface growth process of diamond crystals.