Aligned Self-Assembled Nanostructure by Chemical Force Trigger, Biased Migration, and Oscillatory Hydrogel Growth

Abstract Cells generate pico-to-nanonewton forces through metabolic circuits and diffusion for downstream processes, including stress fiber assembly and cellular growth. The inherent complexities of the system’s processing, reactivity, and adaptability make it difficult to recapitulate in a synthetic setting. Herein, we compartmentalized the urease-urea feedback-controlled reaction network (FCRN), demonstrating global vs local function adaptability by coupling with peptide self-assembly. Compartmentalized FCRN (c-FCRN) facilitates chemical energy-to-mechanical energy conversion, creating forces on the piconewton scale, allowing nanofiber alignment, akin to what a cell does. The trade-off between multiple microscale interactions in the chemo-material network implies molecular-biased migration resembling chemotactic-like directed motion in synthetic settings, which promotes spatial self-assembly remodelling. Consequently, regulating the reaction-diffusion chemistry, we demonstrate oscillatory hydrogel growth by encasing the c-FCRN with a physical membrane barrier. Furthermore, c-FCRN provides a rudimentary structure-building system to create various complex hydrogel structures, bypassing the 3D printing tools. Thus, the chemo-material network provides proof-of-concept for biomimetic material development by emulating biologically inspired technologies.