The aim of this study was to functionalize the surface of Ce-TZP/Al2O3 dental ceramic with a nano-structured alumina coating to improve resin bonding. A total of 40 densely sintered disc-shaped specimens (15.5 + 0.03 mm in diameter and 2.6 + 0.03 mm thick) were produced from commercially available NANOZIR blocks and randomly divided into 2 groups of 20. Half of the discs in each group received an alumina coating that was fabricated by exploiting the hydrolysis of aluminum nitride (AlN) powder. The coating was characterized using scanning electron microscopy (SEM). The shear bond strength of the self-adhesive luting cement G-cem was then studied for the coated and uncoated surfaces before and after thermocycling (TC). The SEM analysis revealed that the application of an alumina coating to Ce-TZP/Al2O3 ceramics created a highly retentive surface for resin penetration. The resin bond strength to the coated groups was significantly higher than to the uncoated groups, both before and after TC (p ≤ 0,05).