With the rapid development of aerospace technology, the high-quality brazing connection between Si3N4 ceramic and TC4 titanium alloy has become a key factor in advancing the development of aircraft antenna covers. To improve the mechanical strength of the joints, this study used the electrophoretic deposition method to prepare a multi-walled carbon nanotubes-foam copper (MWCNTs-Cuf) composite interlayer and selected the optimal deposition parameters. The most suitable brazing parameters under this interlayer were also determined. The joints’ formation mechanism and fracture mode were revealed to elucidate the synergistic strengthening mechanism of the composite interlayer. The results showed that MWCNTs, based on their phase characteristics, produced high-density dislocations and fine crystal strengthening effects during the brazing cooling process. This effectively resisted the corrosion of the brazing material on the foam copper (Cuf), protected the integrity of the foam copper framework, and exerted the excellent plastic deformation ability of foam copper (Cuf). It reduced the residual stress in the joints, resulting in the highest shear strength of the MWCNTs- Cuf composite interlayer, reaching 96.23 MPa. Compared with only adding Ag-Cu-Ti active brazing filler metal and adding ordinary foam copper interlayer, the shear strength increased by 78.2% and 44.7%, respectively.