Zirconia has recently become one of the most popular dental materials in prosthodontics being used in crowns, bridges, and implants. However, weak bonding strength of dental adhesives and resins to zirconia surface has been a grand challenge in dentistry, thus finding a better adhesion to zirconia is urgently required. Marine sessile organisms such as mussels use a unique priming strategy to produce a strong bonding to wet mineral surfaces; one of the distinctive chemical features in the mussel’s adhesive primer proteins is high catechol contents among others. In this study, we pursued a bioinspired adhesion strategy, using a synthetic catechol primer applied to dental zirconia surfaces to study the effect of catecholic priming to shear bond strength. Catechol priming provided a statistically significant enhancement (p < 0.05) in shear bond strength compared to the bonding strength without priming, and relatively stronger bonding than commercially available zirconia priming techniques. This new bioinspired dental priming approach can be an excellent addition to the practitioner’s toolkit to improve dental bonding to zirconia.