Biomolecule-based piezoelectric nanostructures emerged as a new class of energy-converse materials, and designing tailored piezoelectric amino acid arrays is essential to achieve efficient electrical–mechanical coupling and fulfill their application potential. However, the controlled growth of amino acid nanostructures is still challenging due to the limited understanding of their growth mechanism. Herein, we base on the Stranski–Krastanov (S–K) growth mode and propose a mechanism for the growth of ordered amino acid array structures via physical vapor deposition. The growth of vertical valine sheet arrays is examined by changing the substrate temperature, chamber pressure, and source–substrate distance, and a “layer-plus-sheet” growth process is revealed. The modified S–K growth mode is applied to fabricate other amino acid nanostructures like leucine and isoleucine. The growth mode not only explains the formation of uniform and controllable morphology of amino acid structures but also leads to the significant enhancement of their piezoelectric properties. The maximal effective piezoelectric constant of valine sheets is 11.4 pm V–1, which approaches its highest predicted value. The output voltage of the valine array-based nanogenerator is ∼4.6 times the output voltage of the valine powder-based nanogenerator. This work provides new insights into the growth mechanism of ordered piezoelectric amino acid arrays, making them promising candidates for applications in wearable or implantable electronic devices.

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