Titanium materials have been functionalized with biomolecules as a modern strategy to incorporate bioactive motifs that will expand and improve their biomedical applications. Here, we have biofunctionalized biomaterials based on zirconia of much interest for dentistry: the widely used bioceramic 3Y-TZP and a newly developed 3Y-TZP/Ti biocermet. The biosurfaces were activated, silanized, and functionalized with coatings made of oligopeptides. Surface activation by plasma or alkaline-etching was optimized. The surfaces were coated by tethering a purposely-designed RGD-containing peptide. We selected this oligopeptide as a model peptide to validate the effectiveness of the biofunctionalization process. Successful treatments after each step of the process were assessed by surface physical and chemical characterization with water contact angles and XPS, respectively. Coatings' stability was evaluated after 2h sonication in water. Pre-osteoblasts adhesion on the functionalized surfaces was also studied. 10-min air-plasma treatment effectively activated all types of materials with no detrimental effects on the material structure and hardness. Nitrogen XPS-peak confirmed that RGD-peptides were chemically-attached on the silanized samples. This was further confirmed by visualizing the functionalized surfaces with flourescence-labelled RGD-peptides before and after ultrasonication. Furthermore, RGD-functionalized surfaces significantly enhanced osteoblast adhesion on all types of substrates, which demonstrated their successful bioactivation. We successfully developed stable functional biocoatings on zirconia and biocermets made of oligopeptides. Surface bioactivation of zirconia-containing components for dental implant applications will enable their improved clinical performance by incorporating signalling oligopeptides to accelerate osseointegration, improving permucosal sealing, and/or incorporating antimicrobial properties to prevent peri-implant infections.