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This paper reviews our recent work on development of Co-Cr-based longitudinal magnetic recording media through the point of view of thermodynamics. It focuses on our experimental finding on the miscibility gap in the fcc α-Co phase region of the Co-Cr binary system, and on the predictions on the improvements of magnetic properties of many Co-Cr-Z ternary systems by thermodynamic computing on the basis of the newly-assessed Co-Cr binary thermodynamic parameters. Good agreement in the phase separation behavior of many Co-Cr-Z (Z=Pt, Ta, Ge)alloy systems between the calculation and the experiments has been achieved, as discussed in detail in the full paper.By the same token, many other elements, such as Ir, P, B, Mo, Zr, Nb, have been predicted to improve the magnetic grain isolation of the potential Co-Cr-Z multicomponent magnetic recording media in the future.