Nature excels in both self-healing and 3D shaping; for example, self-healable human organs feature functional geometries and microstructures. However, tailoring man-made self-healing materials into complex structures faces substantial challenges. Here, we report a paradigm of photopolymerization-based additive manufacturing of selfhealable elastomer structures with free-form architectures. The paradigm relies on a molecularly designed photoelastomer ink with both thiol and disulfide groups, where the former facilitates a thiol-ene photopolymerization during the additive manufacturing process and the latter enables a disulfide metathesis reaction during the selfhealing process. We find that the competition between the thiol and disulfide groups governs the photocuring rate and self-healing efficiency of the photoelastomer. The self-healing behavior of the photoelastomer is understood with a theoretical model that agrees well with the experimental results. With projection microstereolithography systems, we demonstrate rapid additive manufacturing of single-and multimaterial self-healable structures for 3D soft actuators, multiphase composites, and architected electronics. Compatible with various photopolymerization-based additive manufacturing systems, the photoelastomer is expected to open promising avenues for fabricating structures where free-form architectures and efficient self-healing are both desirable.

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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.

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