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TiAl alloys provide a significantly higher creep resistance at high temperatures. However, the low ductility of these alloys at room temperature is considered as a drawback when used as a turbine blade coating material. One way to increase the ductility is by introducing solutes in the chemical composition of TiAl. Surprisingly, a ductility promotion can be achieved through a phase transition from L10 to B2 phase when the concentrations of Mo, W, and Cu are about 12, 11 and 12.5 at.%, respectively, while there is no phase transformation for TiAl with the presence of Zn. This study will tackle the reason of this behavior by analyzing the enthalpy of formation, mechanical and thermodynamic properties, and electronic structure by performing first‐principles calculations.