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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.