Nanowires (NWs) are among the most studied nanostructures as they have numerous promising applications thanks to their various unique properties. Furthermore, the properties of NWs can be tailored during synthesis by introducing structural defects such as nano‐twins, periodic polytypes, and kinks, i.e., abrupt changes in their axial direction. Here, this work reports for the first time the postsynthesis formation of such defects, achieved by exploiting a peculiar plasticity that may occur in nanosized covalent materials. Specifically, in this work the authors found that single‐crystal CuO NWs can form double kinks when subjected to external mechanical loading. Both the microscopy and atomistic modeling suggest that deformation‐induced twinning along the plane is the mechanism behind this effect. In a single case the authors are able to unkink a NW back to its initial straight profile, indicating the possibility of reversible plasticity in CuO NWs, which is supported by the atomistic simulations. The phenomenon reported here provides novel insights into the mechanisms of plastic deformation in covalent NWs and offers potential avenues for developing techniques to customize the shape of NWs postsynthesis and introduce new functionalities.