The dual-wire electron beam-directed energy deposition (EB-DED) process presents considerable advantages for fabricating titanium aluminide (TiAl) alloys via in situ reactions between Ti and Al. However, variations in the thermophysical properties of pure Ti, pure Al, and TiAl alloys pose challenges in achieving consistent droplet transition behavior and uniform chemical composition. This study explored the effects of wire feeding modes on the forming quality of TiAl alloys and droplet transition behaviors and discussed compositional homogenization and elemental evaporation in TiAl alloy components. Both single-side and double-side feeding modes were utilized, and the electron beam directly melted the Ti wire in the double-side mode, thereby achieving superior surface morphology. Random disturbances and suboptimal wire feeding angles led to the wires deviating from the electron beam center and then being inserted into or passing through the molten pool, thereby degrading the forming quality. By positioning the Al wire tip beneath the Ti wire tip, a common droplet emerged as the Ti droplets melted the Al wire. The droplet transition behavior was regulated by the distance between the wire tips and component surfaces, achieving a liquid bridge transition at distances ranging from 0.75 to 5.82 mm. Although the droplet composition was generally uniform owing to elemental evaporation, the fluctuations among the droplets exceeded those observed in the as-deposited components. The extensive molten pool and keyhole effect enhanced compositional homogenization within the TiAl alloy components. During the deposition process, the evaporation rate of Al surpassed that of Ti due to its higher saturation vapor pressure, consequently yielding a lower actual Al content. The loss rate of Al initially decreased and then increased as the calculated Al content increased, which was influenced by the Al content in the molten pool and temperature variations. This research advances the fundamental understanding of TiAl alloy fabrication via in situ reactions and contributes to the development of the EB-DED process.