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Abstract Extrusion 3D‐printing of biopolymers and natural fiber‐based biocomposites enables the fabrication of complex structures, ranging from implants' scaffolds to eco‐friendly structural materials. However, conventional polymer extrusion requires high energy consumption to reduce viscosity, and natural fiber reinforcement often requires harsh chemical treatments to improve adhesion. We address these challenges by introducing a sustainable framework to fabricate natural biocomposites usingChlorella vulgarismicroalgae as the matrix. Through bioink optimization and process refinement, we produced lightweight, multifunctional materials with hierarchical architectures. Infrared spectroscopy analysis reveals that hydrogen bonding plays a critical role in the binding and reinforcement ofChlorellacells by hydroxyethyl cellulose (HEC). As water content decreases, the hydrogen bonding network evolves from water‐mediated interactions to direct hydrogen bonds between HEC andChlorella, enhancing the mechanical properties. A controlled dehydration process maintains continuous microalgae morphology, preventing cracking. The resulting biocomposites exhibit a bending stiffness of 1.6 GPa and isotropic heat transfer and thermal conductivity of 0.10 W/mK at room temperature, demonstrating effective thermal insulation. These characteristics makeChlorellabiocomposites promising candidates for applications requiring both structural performance and thermal insulation, offering a sustainable alternative to conventional materials in response to growing environmental demands. 

Abstract Inspired by the recent success of buckling‐induced reconfigurable structures, a new class of deployable systems that harness buckling of curved beams upon a rotational input is proposed. First, experimental and numerical methods are combined to investigate the influence of the beam's geometric parameters on its non‐linear response. Then, it is shown that a wide range of deployable architectures can be realized by combining curved beams. Finally, the proposed principles are used to build deployable furniture such as tables and lamp shades that are flat/compact for transportation and storage, require simple or no assembly, and can be expanded by applying a simple rotational input.