International Journal of Molecular Sciences, vol.22, no.12, 2021 (SCI-Expanded)
© 2021 by the authors. Licensee MDPI, Basel, Switzerland.Resin‐based composite materials have been widely used in restorative dental materials due to their aesthetic, mechanical, and physical properties. However, they still encounter clinical shortcomings mainly due to recurrent decay that develops at the composite‐tooth interface. The low‐viscosity adhesive that bonds the composite to the tooth is intended to seal this interface, but the adhesive seal is inherently defective and readily damaged by acids, enzymes, and oral fluids. Bacteria infiltrate the resulting gaps at the composite‐tooth interface and bacterial by‐products de-mineralize the tooth and erode the adhesive. These activities lead to wider and deeper gaps that provide an ideal environment for bacteria to proliferate. This complex degradation process mediated by several biological and environmental factors damages the tooth, destroys the adhesive seal, and ultimately, leads to failure of the composite restoration. This paper describes a co‐tethered dual peptide‐polymer system to address composite‐tooth interface vulnerability. The adhesive system incorporates an antimicrobial peptide to inhibit bacterial attack and a hydroxyapatite‐binding peptide to promote remineralization of damaged tooth structure. A designer spacer sequence was in-corporated into each peptide sequence to not only provide a conjugation site for methacrylate (MA) monomer but also to retain active peptide conformations and enhance the display of the peptides in the material. The resulting MA‐antimicrobial peptides and MA‐remineralization peptides were copolymerized into dental adhesives formulations. The results on the adhesive system composed of co‐tethered peptides demonstrated both strong metabolic inhibition of S. mutans and localized calcium phosphate remineralization. Overall, the result offers a reconfigurable and tunable peptide-polymer hybrid system as next‐generation adhesives to address composite‐tooth interface vulnera-bility.