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Tetragonality has a remarkable influence on the material properties of steels. For example, the shape memory effect is improved by increasing the tetragonality of martensite in Fe-based shape memory alloys. This is because high tetragonality produces thin plate martensites, the mobility of the austenite/martensite interface is increased with increasing tetragonality, and the shape memory effect is improved. Ohtsuka and Kajiwara1) reported that the addition of carbon to a FeNiCoAl alloy coupled with aging treatments increases the First-principles Calculation of Effects of Carbon on Tetragonality and Magnetic Moment in Fe–C System