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The focus of this chapter is the use of bio-inspired, bioengineered or biomimetic systems that find tremendous application in tissue engineering, amongst other applications. Essentially, such systems either have a biological component integrated into the material component or materials that have been designed based on natural or synthetic smart materials. In particular, the chapter will review the use of bio-inspired hierarchical nanocomposites as stimuli-triggered drug deliverable scaffolds in 3-D/4-D-bioprinting, tissues regeneration, vascularization, and biological coatings.

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