Abstract
Medical plastic-appliance-based healthcare services, especially in dentistry, generate tremendous amounts of plastic waste. Given the physiological features of our mouth, it is desirable to substitute dental care plastics with viscoelastic and antimicrobial bioplastics. Herein, we develop a medical-grade and sustainable bioplastic that is viscoelastic enough to align the tooth positions, resists microbial contamination, and exhibits recyclable life cycles. In particular, we devise a molecular template involving entanglement-inducing and antimicrobial groups and prepare a silk fibroin-based dental care bioplastic. The generated compactly entangled structure endows great flexibility, toughness, and viscoelasticity. Therefore, a satisfactory orthodontic outcome is accomplished, as demonstrated by the progressive alignment of male rabbit incisors within the 2.5 mm range. Moreover, the prepared bioplastic exhibits resistance to pathogenic colonization of intraoral microbes such as Streptococcaceae and Veillonellaceae. Because the disentanglement of entangled domains enables selective separation and extraction of the components, the bioplastic can be recycled into a mechanically identical one. The proposed medical-grade and sustainable bioplastic could potentially contribute to a green healthcare future.