Copolymers with varying compositions of catechol methacrylate, MPC, and MAA were synthesized and evaluated for their ability to form antifouling coatings on glass and hydroxyapatite. In the presence of dopamine, thin coatings (∼10 nm) were successfully formed using copolymers 3A–E and 4B–C on glass and hydroxyapatite, whereas, without dopamine, the copolymers formed robust coatings on hydroxyapatite. All copolymer coatings demonstrated strong antifouling properties against E. coli and S. oralis. Most notably, copolymer coatings of 3A–E and 4B–C (without dopamine) on hydroxyapatite significantly reduced the adhesion of S. oralis when evaluated under a variety of conditions, including with a static assay, in the presence of an anionic surfactant, in a swallow test, and in a model mouthwash assay. Copolymers 3A–E reduced the adhesion of S. oralis by more than 85% compared to a bare hydroxyapatite surface in the static assay. This work indicates that this class of functional copolymers can form self-adhesive, antifouling coatings, which we anticipate being applicable in oral care applications, as well as more broadly in the areas of bio-interface adhesion.