Ti6Al4V alloy and ZrO2 ceramic have similar application fields and complementary properties. Brazing connections can broaden the application range. When using sealing glass with good air tightness, good electrical insulation, and low connection temperature to connect, the solder is difficult to wet on the metal surface. The traditional method is to oxidize the surface of the alloy at a high temperature, but the film is not uniform and the treatment time is long. In this study, nanosecond laser surface treatment was used as a prewelding pretreatment method to form a micro-nano structure on the surface and perform oxidation treatment. It is particularly important to select the brazing process. After the laser parameters and processing times were determined, the effects of different welding temperatures and holding times on the properties of the joints were compared, and it was found that there were regular changes. Finally, it is concluded that the maximum shear strength is 46 MPa when the welding temperature is 650 °C and the holding time is 30 min. Under this process, the performance of the joint significantly improved under the dual effects of mechanical bonding and metallurgical bonding. This study provides a new idea for the connection of metal and ceramic and has reference value for the selection of the brazing process.