We investigated ultrasonic welding (USW) of pure α-Ti sheets, which exhibited an insufficient weldability due to the extensive formation of cracks caused by sliding friction during the USW. To overcome this issue, an α/β/α heterogeneous interfacial microstructure was designed by introducing a thin Fe interlayer, a beta stabilizer, between α-Ti sheets. The diffusion of Fe interlayers triggered the formation of a continuous β-Ti thin layer (⁓1–2 μm) without Fe–Ti intermetallics near the bonding interface after USW. The continuous thin β-Ti layer exhibited a significant improvement in the joining of the brittle α-Ti, where the bonding strength was increased from 350 to 1700 N. This study provides a potential approach to design an interfacial microstructure that promotes the formation of a deformable phase, overcoming the inherent brittleness of hexagonal close-packed metals and enabling production of strong joints.