The aim of this study was to assess the shear bond strength and durability between plasma-pretreated and polydopamine (PDA)-coated zirconia and titanium. Four groups were prepared according to the different surface treatments (untreated ZrO₂, plasma-pretreated ZrO₂, PDA-coated ZrO₂, and plasma-pretreated and PDA-coated ZrO₂ (PP+PDA-ZrO₂). The surface topography and roughness, contact angle, and elemental analysis of the coatings of the four groups were investigated, and the bond strength and durability of the specimens were evaluated based on shear bond strength and thermocycle tests. Physical and chemical characterization results confirmed that PDA coatings can be successfully formed on zirconia substrates. The roughness and hydrophilicity were significantly higher in the PP+PDA-ZrO₂ group_, which demonstrated better shear bond strength and durability between zirconia and titanium. The plasma pretreatment of zirconia substrates can enhance the stability of the PDA coating layer, and hybrid surface modifications can provide several bonding advantages for clinical use.