Biofabrication Strategies for Biodegradable Piezoelectric Interfaces Toward Bioelectronic Systems

ABSTRACT Piezoelectricity enabled direct interconversion of mechanical and electrical signals underpin a broad range of biomedical and electronic technologies. However, state‐of‐the‐art ceramic and fluoropolymer piezoelectrics remain fundamentally mismatched with biological systems due to mechanical rigidity, toxicity, limited degradability, and regulatory constraints. In contrast, biodegradable and bio‐derived piezoelectric materials offer intrinsic electromechanical activity combined with mechanical compliance, biocompatibility, and environmental sustainability. Recent advances reveal that modest intrinsic piezoelectric coefficients are not a fundamental limitation; rather, various bio‐fabrication strategies amplify molecular symmetry breaking, hierarchical organization, and interfacial engineering which can collectively enable highly efficient electromechanical transduction in bio‐organic systems. This review examines the emerging paradigm of bio‐responsive piezoelectric interfaces, spanning amino acids, peptides, proteins, polysaccharides, and engineered biodegradable molecular crystals. We integrate insights from density functional theory, molecular dynamics, and data‐driven materials screening with advances in molecular engineering, supramolecular assembly, electric and magnetic field‐, mechano‐, and thermally assisted fabrication. Additional focus is placed on symmetry control, hydrogen‐bond networks, cooperative lattice mechanics, and interface‐mediated polarization. Finally, we highlight transformative applications in self‐powered bioelectronics, while outlining key challenges and probable solutions in materials barrier, processing limitations, quantitative characterizations and bioelectronics devices. These perspectives establish bio‐piezoelectric materials for sustainable electromechanical systems.