Background: currently applied surface treatments for zirconia bonding may create undesired microcracks and surface flaws. The aim of the present study was to evaluate the efficacy of alternative surface treatments on the shear bond strength of high translucency zirconia to 10-Methacryloyloxydecyl dihydrogen phosphate (MDP)-containing resin-based cement. Methods: fifty disk-shaped specimens (10 mm × 5 mm) were fabricated from a commercial yttria-stabilized zirconia with 5 mole% yttrium oxide tetragonal zirconia polycrystal (5Y-TZP), and underwent air-abrasion with alumina particles (50 μm-AL50 and 90 μm-AL90), glass beads (GB 10–60 μm), and ablation with femtosecond laser (FEMTO). Shear bond strength was evaluated with a universal testing machine under a crosshead speed of 0.5 mm/min until fracture. Fracture type was evaluated with an optical stereomicroscope. Differences among groups were evaluated by one-way ANOVA and Bonferroni pairwise comparison tests (p < 0.05). Results: the highest shear bond strength values were presented by the laser treated group (23.97 ± 3.7 MPa). No statistically significant differences were found among the Cl, Al50, Al90 and FEMTO groups. The lowest mean value was presented by the glass-beads treated group (11.93 ± 2.88 MPa) which was significantly lower compared to all other groups (p < 0.001). Conclusions: under the limitations of this in vitro study, femtosecond laser treatment of High-translucent monolithic zirconia (HTZ) ceramics is a promising alternative method for the mechanical retention of resin cements.