Using the methods of scanning and transmission electron microscopy, the features of the structural-phase state of a vanadium alloy of the V–Cr–Ta–Zr system after a combined treatment, which consisted in cyclic alternation of thermomechanical and chemical-heat treatments, were studied. The values of yield strength and ductility of the V–Cr–Ta–Zr alloy were determined, depending on the stabilization and test temperatures. It was established that, after the combined treatment, the structural-phase state of the V–Cr–Ta–Zr alloy was composite, in which the joint implementation of dispersion and substructural strengthening ensured the formation of a gradient grain structure with a polygonal state, the elements of which were fixed by nanosized ZrO2 particles characterized by a high thermal stability. Such modification of the microstructure was accompanied by an increase in the high-temperature strength and a shift in the upper limit of the temperature stability interval towards high temperatures, of up to 900 °C. It was assumed that the polygonal state inside the grains contributed to the implementation of cooperative mechanisms of the dislocation–disclination type, which ensured the accommodation of the material in the “high-strength state” under loading.