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This study proposes a method to enhance the airtightness of the joint between the ZrO₂ and Crofer alloy using coating technology. With the aid of vacuum sputtering technology, a titanium–copper alloy layer with a thickness between 1.5 μm and 6 μm was first deposited on the surface of ZrO₂ and Crofer, respectively. The chemical composition of the deposited reaction layer was 70.2 Cu and 29.8 Ti in at%. Then, using silver as the base material in the reactive air brazing (RAB) process, we explore the use of this material design to improve the microstructure and reaction mechanism of the joint surface between ceramics and metal, compare the effects of different pretreatment thicknesses on the microstructure, and evaluate its effectiveness through air tightness tests. The results show that a coating of Cu-Ti alloy on the ZrO₂ substrate can significantly improve bonding between the Ag filler and ZrO₂. The Cu-Ti metallization layer on the ZrO₂ substrate is beneficial to the RAB. After the brazing process, the coated Cu-Ti layers form suitable reaction interfaces between the filler, the metal, the filler, and the ceramic. In terms of coating layer thickness, the optimized 3 μm coated Cu-Ti alloy layer is achieved from the experiment. Melting and dissolving the Cu-Ti coated layer into the ZrO₂ substrate results in a defect-free interface between the Ag-rich braze and the ZrO₂. The air tightness test result shows no leakage under 2 psig at room temperature for 28 h. The pressure condition can still be maintained even under high-temperature conditions of 600 °C for 24 h.