During the laser-based additive manufacturing (via the DED route) of Ti64 alloy the growth of columnar β-grains along the built direction observed in the resulting microstructure leads to various mechanical anisotropy limiting its functionality.  Many studies have addressed this issue by the addition of various β-phase stabilizing elements to the Ti64 alloy system, as it promotes the columnar to equiaxed transition (CET). The addition of Fe as a β-phase stabilizer has been studied in various literature, which remarkably improves mechanical strength by promoting CET while sacrificing ductility.  In this study, we have attempted the addition of Co and Fe to the Ti64-alloy system via a laser processing route to improve the elongation properties of the Ti64-Fe system. The Ti64-Fe-based alloy systems, with and without the addition of Co have been studied through the non-equilibrium solidification simulation using CALPHAD methods, where no undesirable intermetallic phase formation is noticed. The obtained microstructures also show very fine α-lathes with equiaxed β-grains for both the case of the laser-processed alloys. A (45-50) % improvement in the hardness value is observed for both cases, where a reduction of elastic modulus for the case of Co addition shows the effectiveness of Co in reducing the stiffness of the Ti64-Fe alloy system. Hence, the addition of Co as a substitutional alloying element improves the elongation properties of the Ti64-Fe system without affecting its strength. This alloy system can be further studied to design a β-phase strengthened Ti64-based alloy system with improved strength and ductility via additive manufacturing routes (DED).