This study aimed to evaluate the effects of different surface preparation techniques on the surface microstructure, the shear bond strength (SBS) between zirconia and an MDP-containing light-cured veneer adhesive system, and the adhesive failure mode. Sixty-four zirconia specimens were divided into four groups based on surface preparation methods (n = 16), including zirconia sandblasting (ZSB), zirconia vitrification or glaze-on (ZVG), zirconia surface architecture technique (ZSAT), and ZSAT-ZVG combined technique (ZSATVG) groups. Sixteen lithium disilicate specimens prepared by etching with hydrofluoric acid (HF) were used as a positive control group (LDE). Surface roughness measurement and scanning electron microscopy (SEM) evaluation were performed before and after surface preparation. All specimens were then bonded with an MDP-containing light-cured adhesive system, followed by SBS testing and adhesive failure mode analysis. The ZVG and ZSATVG groups showed the greatest differential roughness value and microscopic irregularities, while the ZSAT and LDE groups had the least surface change but the most micromechanical retentive structures for resin infiltration. SBS values were significantly different among groups (p < 0.001) with the highest SBS observed in the ZSAT group, followed by the ZSB group, LDE group, ZSATVG group, and lastly, the ZVG group. There was a statistically significant difference in failure types among the surface preparation groups (p < 0.001). The ZSAT group had the highest frequency of mixed failure, followed by the ZSB group, LDE group, and the ZSATVG and ZVG groups. Establishing direct micromechanical retention within zirconia itself yields a higher bond strength than indirect micromechanical retention within a glass ceramic layer.