Ferritic-martensitic steels alloyed with Cr and Ni are promising structural materials for the nuclear and thermonuclear power industry. Under the influence of neutron irradiation degradation of the plastic properties of these materials takes place as a result of the generation of extended defects such as dislocation loops, and the formation of new phases (precipitates). In this work the atomistic computer simulation of thermodynamic processes of the precipitation of alloying elements is carried out using the newest model of ternary Fe–Ni–Cr bcc (body-centered cubic) alloys and the Metropolis Monte Carlo method in combination with the method of classical Molecular Dynamics. The composition and microstructure of Cr–Ni clusters formed in defect-free alloys and alloys containing dislocation loops, depending on the temperature and concentrations of Ni and Cr, are studied. An increase in the Ni solubility limit in the presence of dislocation loops by 100–200 K, depending on the Ni concentration, is detected. The synergetic effect of Ni and Cr segregation near dislocation loops in ternary alloy is established: the presence of Ni weakens Cr segregation, whereas Cr can either attenuate or amplify Ni segregation depending on the concentration of Ni in the alloy, the temperature and the type (Burgers vector) of loop. In general, in ternary Fe–Cr–Ni alloys, the total segregation effect is less pronounced than in binary Fe–Ni and Fe–Cr alloys.