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Synthetic biology applies genetic tools to engineer living cells and organisms analogous to the programming of machines. In materials synthetic biology, engineering principles from synthetic biology and materials science are integrated to redesign living systems as dynamic and responsive materials with emerging and programmable functionalities. In this Review, we discuss synthetic-biology tools, including genetic circuits, model organisms and design parameters, which can be applied for the construction of smart living materials. We investigate non-living and living self-organizing multifunctional materials, such as intracellular structures and engineered biofilms, and examine the design and applications of hybrid living materials, including living sensors, therapeutics and electronics, as well as energy-conversion materials and living building materials. Finally, we consider prospects and challenges of …