Rational Design of Bioinspired Nucleobase‐Containing Polymers as Tough Bioplastics and Ultra‐Strong Adhesives

Abstract The development of polymeric materials from bio‐based feedstocks is highly urgent due to growing environmental concerns and the rapid depletion of limited fossil resources. However, bio‐based polymeric materials usually possess only moderate performance, drastically undermining their potential applicability. Herein, bioinspired nucleobase‐containing polymers with eminent toughness and outstanding adhesive properties by harnessing the complementary hydrogen‐bonding (H‐bonding) interactions are developed. Efficient thiol‐ene polymerization is carried out to produce the nucleobase‐functionalized homopolymers and statistical copolymers. In contrast to the individual homopolymers, the supramolecular mixtures of the homopolymers display much better energy dissipation and damping capacity on account of intermolecular complementary H‐bonding interactions. More remarkably, the nucleobase‐containing copolymers possessing both inter‐ and intramolecular complementary H‐bonding interactions exhibit outstanding toughness as high as 73.8 MJ m −3 . In addition to the outstanding mechanical properties, the unique interfacial adhesive propensity of nucleobases endows the polymeric materials with an ultra‐strong adhesion strength as high as 16.2 MPa. This work represents an important and universal bioinspired strategy to construct robust polymeric materials by rationally designing both inter‐ and intramolecular H‐bonding networks.