This paper addresses how solute segregation and phase separation evolves the intrinsic growth stresses for Fe-4Cr and Fe-16Cr (at.%) nanocrystalline films. Ambient temperature deposition resulted in both alloys exhibiting a near equivalent tensile stress though the average grain sizes were approximately 50 nm and 100 nm respectively. Upon heating during deposition to 523 K and 673 K, the tensile stress was reduced in each film and it eventually became compressive for the higher deposition temperature. Interestingly, the Fe-16Cr film, at the higher heating temperature, diverted from the steady state compressive stress towards a tensile stress after approximately 150 nm of growth. The collective stress evolution of these films is discussed in terms of their phase separation, which can include spinodal deposition, as a function of Cr content and processing temperature. It was found that Cr acted as a grain refiner which appeared to dominate the film microstructure and associated stress response.