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.