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The mechanical properties of engineering structures continuously weaken during service life because of material fatigue or degradation. By contrast, living organisms are able to strengthen their mechanical properties by regenerating parts of their structures. For example, plants strengthen their cell structures by transforming photosynthesis-produced glucose into stiff polysaccharides. In this work, we realize hybrid materials that use photosynthesis of embedded chloroplasts to remodel their microstructures. These materials can be used to three-dimensionally (3D)-print functional structures, which are endowed with matrix-strengthening and crack healing when exposed to white light. The mechanism relies on a 3D-printable polymer that allows for an additional cross-linking reaction with photosynthesis-produced glucose in the material bulk or on the interface. The remodeling behavior can be suspended by freezing chloroplasts, regulated by mechanical preloads, and reversed by environmental cues. This work opens the door for the design of hybrid synthetic-living materials, for applications such as smart composites, lightweight structures, and soft robotics. 

Abstract Living creatures are continuous sources of inspiration for designing synthetic materials. However, living creatures are typically different from synthetic materials because the former consist of living cells to support their growth and regeneration. Although natural systems can grow materials with sophisticated microstructures, how to harness living cells to grow materials with predesigned microstructures in engineering systems remains largely elusive. Here, an attempt to exploit living bacteria and 3D‐printed materials to grow bionic mineralized composites with ordered microstructures is reported. The bionic composites exhibit outstanding specific strength and fracture toughness, which are comparable to natural composites, and exceptional energy absorption capability superior to both natural and artificial counterparts. This report opens the door for 3D‐architectured hybrid synthetic–living materials with living ordered microstructures and exceptional properties.