The molecular dynamics method was used to study the structure formation during austenite nanoparticles crystallization in the presence of carbon impurities. The paper describes the dependence of the melt cooling rate, particle size, concentration of carbon atoms in the particle on the resulting structure features during crystallization and temperature of the crystallization onset. Formation of the nanocrystalline structure of nanoparticles can be controlled by varying the cooling rate and introducing a carbon impurity: at a cooling rate above 1013 K/s in the model used, crystallization did not have time to occur; at a rate below 5·1012 K/s, the austenite particle crystallized to form a nanocrystalline structure. At the same time, with a decrease in the cooling rate, a decrease in the density of defects in the final structure was observed. At a rate of 5·1011 K/s or less, crystallization of carbon-free particles took place with the formation of low-energy grain boundaries (with a high density of conjugate nodes: special boundaries, twins). The crystallization temperature during cooling at a rate below 1012 K/s is inversely proportional to the particle diameter: as the particle size decreases, the proportion of free surface increases, which leads to a decrease in the probability of crystalline nuclei formation. In addition, the crystallization temperature increases with a decrease in the cooling rate. The introduction of a carbon impurity led to a decrease in the crystallization temperature of nanoparticles: in the presence of 10 at. %. As a percentage of carbon, it decreased by about 200 K for particles of different sizes. Carbon atoms often formed clusters consisting of several carbon atoms. Such clusters distorted the resulting crystal lattice of metal around them, preventing crystallization. In the presence of a carbon impurity, the final structure of the crystallized particles contained a higher density of grain boundaries and other defects. Carbon atoms, especially clusters of them, were fixed mainly at grain boundaries and triple joints.