Ti−6Al−4V/Al7050 joints were fabricated by a method of insert molding and corresponding interfacial microstructure and mechanical properties were investigated. The interfacial thickness was sensitive to holding temperature during the first stage, and a good metallurgical bonding interface with a thickness of about 90 µm can be obtained at 750°C. X-ray diffraction, transmission electron microscopy, and thermodynamic analyses showed that the interface mainly contained intermetallic compound TiAl 3 and Al matrix. The joints featured good mechanical properties, i.e., shear strength of 154 MPa, tensile strength of 215 MPa, and compressive strength of 283 MPa, which are superior to those of joints fabricated by other methods. Coherent boundaries between Al/TiAl 3 and TiAl 3 /Ti were confirmed to contribute to outstanding interfacial mechanical properties and also explained constant fracture occurrence in the Al matrix. Follow-up studies should focus on improving mechanical properties of the Al matrix by deformation and heat treatment.