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On the basis of the recently proposed physically-based segmented model, the descriptions for the Gibbs energy of pure Cr and Ta down to 0 K were first established. After that, a thermodynamic re-assessment of the binary Cr–Ta system down to 0 K was then performed by taking into account all the critically reviewed experimental phase equilibria and thermodynamic properties. Especially, the experimental heat capacities of Cr2Ta at low temperatures ignored in previous assessments were utilized in the present assessment. The calculated phase equilibria and thermodynamic properties according to the presently obtained thermodynamic descriptions of the binary Cr–Ta system agree well with most of the experimental data, and show better agreement than the previous assessment.