This thrust employs a fundamental materials science approach to study stimuli-responsive smart biomaterials and cell-free bioprogrammable materials, addressing gaps in the bioinspired materials field. It integrates experimental investigations with computer simulations to probe three phase transition phenomena under different stimuli: (a) pH-triggered conformational change in polydiacetylene-peptide, (b) glutathione-stimulated morphological change in polyurethane polymer nanoparticles, and (c) AC magnetic field-activated phase transition, from hydrophobic to hydrophilic, in polymeric nanocomposites containing superparamagnetic iron oxide nanoparticles. Additionally, shape-morphing 3D materials with programmable morphologies and motions will be synthesized, mimicking living tissues. These advancements aim to develop novel polymeric biomaterials and bioinspired materials for applications such as drug delivery, tissue repair and regeneration, and related biomedical uses.