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Abundant experimental diffusion data in two Co-base binary systems, that is, Co-Ni and Co-Fe, have been assessed to develop the atomic mobility for the face-centered cubic (fcc) phase of the two binaries. The general agreement is obtained by comprehensive comparisons made between the calculated and experimental diffusion coefficients. The developed mobility database, in conjunction with the CALPHAD-type thermodynamic description, has been successfully used to simulate such typical experimental interdiffusion phenomena as the concentration profiles, the microstructural stability of the Kirkendall plane, and the lattice plane displacement.