Piezoelectric biomaterials are intrinsically suitable to convert mechanical energy to electrical output and achieve electricity generation, in vivo/in vitro real-time monitoring, and sensing in biological systems. However, the inability to fabricate piezoelectric bio-materials with excellent piezoelectricity, full biodegradability, and good biocompatibility remains a challenge toward practical applications. As a solution, we present a bio-piezoelectric thin film with macroscopic piezoelectric output, high stability, fast response ability, flexibility, biocompatibility, and biodegradability based on nascent silk nanoribbons (SNRs) with high silk II-type structure. The solvent systems influence the meso/nanostructure and the piezoelectric performance of silk materials. Compared with other silk materials, the SNR fabricated by 2,2,6,6-tetramethylpiperidine-1-oxyl oxidation system (T-SNR) maintains higher silk II-type structure and more stable crystalline structure. The T-SNR film possesses electrostriction effect without electrical poling treatment. It presents an apparent piezoelectric constant (d33) of 7.7 pm/V and a piezoelectric voltage coefficient (g33) of 0.58 Vm/N, such values are superior to most reported bio-films. The piezoelectric T-SNR film can realize in vivo/in vitro real-time monitoring, sensing, and self-power ability. With its natural compatibility and degradability, the T-SNR film exhibits the potential for various implantable and wearable applications and may enable the development of fully biodegradable transient electromechanical devices.
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