Nanocrystalline Cr-Fe-Ni thin films libraries are prepared by radio frequency magnetron sputter codeposition on Al2O3 substrates. The variation in distance from different points on the substrate to the three sputter sources produces a spread in composition in the films. Synchrotron radiation is used to analyze composition, crystallographic phase, and grain size as a function of sample position, both as-deposited and after annealing. In addition to three equilibrium phases (bcc, fcc and sigma-FeCr), a fourth phase is observed which does not correspond to any equilibrium phase in the Cr-Fe-Ni system, but which is consistent with the alpha-Mn structure. The films are initially nanocrystalline; both equilibrium and nonequilibrium phases are observed. Tertiary phase diagrams measured at annealing temperatures of 200-800 degrees C show that the stability of nanocrystalline material against thermal grain growth varies widely with composition, and that the crystallographic phase can be selected to be an appropriate heat treatment. Thus, the approach used here is useful for technologies such as magnetic recording media where understanding the stability of the nanograin structure is critical. (c) 2005 Elsevier B.V. All rights reserved.