Multiscale Bio-Interfacing Strategies for Engineered Living Materials

The integration of synthetic polymers with biological systems requires overcoming interfacial challenges across multiple scales. We present a comprehensive toolkit for creating dynamic Engineered Living Materials (ELMs) by bridging hydrogels with living cells, decellularized scaffolds, and whole plants. First, we introduce "plant cyborgs" by 3D printing stimuli-responsive hydrogels onto decellularized leaf scaffolds. This hybrid system harnesses the strain mismatch between the synthetic gel and the natural vascular architecture to achieve programmable shape-morphing in response to thermal and light stimuli. Second, to interface these functional materials with living plants, we developed a hydrogel adhesive capable of forming reversible, dynamic covalent bonds with diverse plant topologies. Finally, at the cellular level, we demonstrate a diffusion-mediated encapsulation strategy that incorporates Synechococcus elongatus into cytotoxic hydrogel precursors. This approach revealed a secreted amidase that autonomously alters the material's mechanical properties over time. Together, these strategies—ranging from cellular encapsulation and scaffold actuation to macroscopic adhesion—establish a versatile platform for next-generation responsive bio-hybrids.