Shape and dimensionality control by ligands is an efficient way to fabricate high-quality perovskite nanocrystals (NCs) with optoelectronic properties. Herein, to realize oriented transformations between different morphologies of CsPbBr3nanocrystals, we conceived of the use of defects and bidentate ligands to synergistically drive the reorientation of CsPbBr3nanocrystals into CsPbBr3nanowires (NWs). By employing aminocaproic acid as the bidentate ligand, CsPbBr3NWs were reconstructed from the CsPbBr3NCs (∼7 nm) with 20-60 nm in width and several micrometers in length, as well as a 527 nm photoluminescence (PL) peak, 59% PL quantum yield, and 98.5 ns PL lifetime. The bidentate ligand-directed anisotropic shape evolution and growth of perovskite NWs from NCs was elucidated by transmission electronmicroscopy and PL studies. The photodetectors fabricated with the reconstructed CsPbBr3NWs displayed a photocurrent enhancement (2.75 × 10-11A) compared with that of the devices based on solution-synthesized NWs (2.28 × 10-11A). The device also showed a short response time, indicating its more sensitive photoelectric response. This process provides a viable approach to engineering diverse morphologies of perovskite nanocrystals for optoelectronic applications.