This paper addresses in situ stress evolution of two-component FexPt1−x, where x spanned 0 to 1, alloy thin films. The stresses of the high-temperature, quenched-in, solid solution phase was determined by in situ wafer curvature measurements during ambient temperature growth. The measured stresses were shown to be compositional dependent and spanned both compressive and tensile stress states. Under specific growth conditions, a “zero-stress” state could be achieved. The alloy stress states did not show any significant stress recovery upon ceasing the deposition, i.e. the stress state during growth was retained in the film. X-ray diffraction, transmission electron microscopy, and atom probe tomography were used to characterize the microstructures of each thin film. The evolution of the stress state with composition is described in terms of a chemical potential term for preferential segregation of one species in the alloy to the grain boundaries.