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Self-assembled biomaterials are made of building blocks that are held together with weak and noncovalent interactions to form well-ordered structures spontaneously. Guided by nature, the architectures built by a self-assembly approach were fabricated with abundant structure variation two-dimensions and three-dimensions endowed with various biofunctions for tissue engineering applications. Beyond natural sources, artificial building blocks were designed and synthesized to achieve better properties not only with structures but also with biomimetic functions. In this work, different classes of self-assembled biomaterials have been reviewed including design concepts, synthetic methods, structures, functions and application issues in tissue engineering. For modern improvements, the stimuli-responsive and in vivo reconstruction properties have also been discussed in this chapter to better understand these fascinating self-assembled biomaterials.

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