This paper describes thermodynamic modeling of the NiAl–CrMoCo system with the calculation of the equilibrium composition and thermodynamic parameters of the system. NiAl-Cr-Mo-Co alloy samples of equiatomic composition, including those with a small addition of zirconium oxide nanoparticles, were obtained by spark plasma sintering of mechanically alloyed powders. It was found that the material had a two-phase structure with wedge-shaped regions enriched in cobalt and molybdenum with a gradient distribution. In addition, in the regions enriched with (Cr, Mo) phase, a lamellar σ phase was found. Fractographic analysis showed a positive effect of the fine-grained wedge-shaped regions on the damping of crack propagation. The alloy with the addition of zirconium oxide nanoparticles had a bending strength and an elastic modulus of 611 MPa and 295 GPa at 25 °C, and 604 MPa and 260 GPa at 750 °C, respectively, when tested in vacuum.