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Despite the considerable potential and significant promise of aluminum scandium nitride (AlScN) ferroelectric materials for neuromorphic computing applications, challenges related to device engineering, along with the considerable structural disorder in thin films grown on various substrates using different vapor synthesis methods, make it difficult to systematically study the structure–property relationship. In this work, we approach such issues from the crystal growth side by successfully growing high-quality single crystal AlScN nanowires through ultra-high vacuum reactive sputtering under high substrate bias and low atomic flux conditions, which leads to simultaneous growth and etching. Characterization of nanowire arrays using X-ray diffraction and transmission electron microscopy shows that the wires are epitaxial single crystals with significantly reduced mosaic spread and predominantly single ferroelectric domains. Moreover, ferroelectric and piezoelectric properties were evaluated using Piezoresponse Force Microscopy. The single crystal AlScN nanowires show an out-of-plane piezoelectric constant d33 that is greater than 20 pm V−1, which is higher than that of pure AlN by a factor of ∼4. [ABSTRACT FROM AUTHOR]