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Hydrogels with the ability to change shape in response to biochemical stimuli are important for biosensing, smart medicine, drug delivery, and soft robotics. Here, a family of multicomponent DNA polymerization motor gels with different polymer backbones is created, including acrylamide‐co‐bis‐acrylamide (Am‐BIS), poly(ethylene glycol) diacrylate (PEGDA), and gelatin‐methacryloyl (GelMA) that swell extensively in response to specific DNA sequences. A common mechanism, a polymerization motor that induces swelling is driven by a cascade of DNA hairpin insertions into hydrogel crosslinks. These multicomponent hydrogels can be photopatterned into distinct shapes, have a broad range of mechanical properties, including tunable shear moduli between 297 and 3888 Pa and enhanced biocompatibility. Human cells adhere to the GelMA‐DNA gels and remain viable during ≈70% volumetric swelling of the gel scaffold induced by DNA sequences. The results demonstrate the generality of sequential DNA hairpin insertion as a mechanism for inducing shape change in multicomponent hydrogels, suggesting widespread applicability of polymerization motor gels in biomaterials science and engineering.

 

Self‐folding broadly refers to the assembly of 3D structures by bending, curving, and folding without the need for manual or mechanized intervention. Self‐folding is scientifically interesting because self‐folded structures, from plant leaves to gut villi to cerebral gyri, abound in nature. From an engineering perspective, self‐folding of sub‐millimeter‐sized structures addresses major hurdles in nano‐ and micro‐manufacturing. This review focuses on self‐folding using surface tension or capillary forces derived from the minimization of liquid interfacial area. Due to favorable downscaling with length, at small scales capillary forces become extremely large relative to forces that scale with volume, such as gravity or inertia, and to forces that scale with area, such as elasticity. The major demonstrated classes of capillary force assisted self‐folding are discussed. These classes include the use of rigid or soft and micro‐ or nano‐patterned precursors that are assembled using a variety of liquids such as water, molten polymers, and liquid metals. The authors outline the underlying physics and highlight important design considerations that maximize rigidity, strength, and yield of the assembled structures. They also discuss applications of capillary self‐folding structures in engineering and medicine. Finally, the authors conclude by summarizing standing challenges and describing future trends.

 

Conventional assembly of biosystems has relied on bottom‐up techniques, such as directed aggregation, or top‐down techniques, such as layer‐by‐layer integration, using advanced lithographic and additive manufacturing processes. However, these methods often fail to mimic the complex three dimensional (3D) microstructure of naturally occurring biomachinery, cells, and organisms regarding assembly throughput, precision, material heterogeneity, and resolution. Pop‐up, buckling, and self‐folding methods, reminiscent of paper origami, allow the high‐throughput assembly of static or reconfigurable biosystems of relevance to biosensors, biomicrofluidics, cell and tissue engineering, drug delivery, and minimally invasive surgery. The universal principle in these assembly methods is the engineering of intrinsic or extrinsic forces to cause local or global shape changes via bending, curving, or folding resulting in the final 3D structure. The forces can result from stresses that are engineered either during or applied externally after synthesis or fabrication. The methods facilitate the high‐throughput assembly of biosystems in simultaneously micro or nanopatterned and layered geometries that can be challenging if not impossible to assemble by alternate methods. The authors classify methods based on length scale and biologically relevant applications; examples of significant advances and future challenges are highlighted.

 

Interfacing nano/microscale elements with biological components in 3D contexts opens new possibilities for mimicry, bionics, and augmentation of organismically and anatomically inspired materials. Abiotic nanoscale elements such as plasmonic nanostructures, piezoelectric ribbons, and thin film semiconductor devices interact with electromagnetic fields to facilitate advanced capabilities such as communication at a distance, digital feedback loops, logic, and memory. Biological components such as proteins, polynucleotides, cells, and organs feature complex chemical synthetic networks that can regulate growth, change shape, adapt, and regenerate. Abiotic and biotic components can be integrated in all three dimensions in a well‐ordered and programmed manner with high tunability, versatility, and resolution to produce radically new materials and hybrid devices such as sensor fabrics, anatomically mimetic microfluidic modules, artificial tissues, smart prostheses, and bionic devices. In this critical Review, applications of small scale devices in 3D hybrid integration, biomicrofluidics, advanced prostheses, and bionic organs are discussed.

 

Changes in structure and function of small muscular arteries play a major role in the pathophysiology of pulmonary hypertension, a burgeoning public health challenge. Improved anatomically mimetic in vitro models of these microvessels are urgently needed because nonhuman vessels and previous models do not accurately recapitulate the microenvironment and architecture of the human microvascular wall. Here, we describe parallel biofabrication of photopatterned self-rolled biomimetic pulmonary arterial microvessels of tunable size and infrastructure. These microvessels feature anatomically accurate layering and patterning of aligned human smooth muscle cells, extracellular matrix, and endothelial cells and exhibit notable increases in endothelial longevity and nitric oxide production. Computational image processing yielded high-resolution 3D perspectives of cells and proteins. Our studies provide a new paradigm for engineering multicellular tissues with precise 3D spatial positioning of multiple constituents in planar moieties, providing a biomimetic platform for investigation of microvascular pathobiology in human disease.