Spider silk and silkworm silk are the most attractive biomaterials with extraordinary mechanical properties created by nature. Besides, chitin, cellulose and polysaccharides are the most abundant natural biomaterials and have been widely used by humans. Elucidating the precise control of the multi-scale structure and dynamics in biomacromolecules, and furthermore, developing biopolymer materials with high performance through multi-scale biomimetic methods, and achieving the high-performance for traditional synthetic polymers are important research topics in polymer science. In this project, multi-scale solid-state NMR in combination with other characterization techniques will be adopted to reveal the micro-phase separation structure and interface in high-performance natural biomaterials, such as the hydrogen bond interaction between water and biomacromolecules, the complex chain motion of the biomacromolecules, evolution of multi-scale structure and dynamics during the stretching process as well as its influence on the mechanical properties in different length and time scales, thus to establish an in-depth understanding of the structure-property relationships of high-performance biomaterials. On the basis of the above work and through multi-scale biomimetic molecular design, we will prepare a series of high-performance biomimetic polymer materials based on biopolymers and synthetic polymer with high density of hydrogen bonds, such as chitosan and multi-block polyurethanes. Our work will promote the fundamental research and industrial applications of high-performance biopolymer and polymer materials of our country.