The hydrogen bonding interactions in BisGMA and urethane dimethacrylate (UDMA) based resins provides positive reinforcement to polymer networks that enhance overall strength. In this study, we are taking the noncovalent interactions involving urethane functionality to an elevated level by preferentially inserting urethane-carboxylate hydrogen bonding interactions and designing novel copolymers that reach near quantitative conversion during a brief ambient temperature photopolymerization. The highly converted polymer also displays extremely high modulus, strength and toughness. The proposed project will investigate the structure-property relationships that allow this unusual combination of polymer properties to coexist while also developing a fundamental understanding of the mechanism by which it occurs. The addition of filler to these interesting resins will provide novel materials with substantially higher performance than existing composites. negligible leachable free monomer and extreme mechanical strength combined with exceptional toughness. Based on the hypothesis of a latent onset of polymeric vitrification following complete conversion, the expectation is that polymerization stress will be quite low, which will be assessed. An unfilled polymer with structure related to the central materials to be developed here demonstrated dramatically increased wear resistance compared to both unfilled and filled commercial dental polymers and even out-performed a lithium disilicate ceramic. Since the self-reinforced polymers involved here offer even greater strength, higher modulus and more extensive toughness and resilience, we anticipate that the filled version of these materials will promote even more impressive wear behavior. As the project progresses, biocompatibility using both direct contact and elution testing will be in place to assure that only viable composite materials will be advanced. A mechanically robust composite that does not leach unreacted monomer because the monomers are fully consumed during polymer network formation has potential to mitigate the current concerns of both composite fracture and secondary caries, which together account for the large majority of failures of resin-based composite restorations. The pilot project proposed here will identify and validate practical candidate materials as a new class of composite restoratives that represent a non-incremental advance in this field upon which the current and future practice of dentistry remains so reliant. The comprehensive nature of the analytical characterization involved here relies on previously peer-reviewed published techniques that meet the challenge of rigor.