Carbon nanofibers (NFs) have been envisioned with broad promising applications, such as nanoscale actuators and energy storage medium. This work reports for the first-time superelastic tensile characteristics of NFs constructed from a screw dislocation of carbon nanocones (NF-S). The NF-S exhibits three distinct elastic deformation stages under tensile, including an initial homogeneous deformation, delamination, and further stretch of covalent bonds. The delamination process endows the NF-S extraordinary tensile deformation capability, which is not accessible from its counterpart with a normal cup-stacked geometry. The failure of NF-S is governed by the inner edges of the nanocone due to the strain concentration, leading to a common failure force for NF-S with varying geometrical parameters. Strikingly, the delamination process is dominated by the inner radius and the apex angle of the nanocone. For a fixed apex angle, the yielding strain increases remarkably when the inner radius increases, which can exceed 1000%. It is also found that the screw dislocation allows the nanocones flattening and sliding during compression. This study provides a comprehensive understanding on the mechanical properties of NFs as constructed from carbon nanocones, which opens new avenues for novel applications, such as nanoscale actuators. (Haifei Zhan) 1 = ( /2) and 1 = ( /2), respectively. Considering the close packing morphology, i.e., the distance between each layer equals to the graphite distance (b = 3.35 Å), the effective height or length of the nanofiber can be approximated as ℎ 1 = ( − 1) /sin ( 2 ⁄ ). Thus, the cross-section and volume of the nanofiber can be approximated as 1 = ( = − = ) sin( 2 ⁄ ) = , and 1 = ( − 1)( = − = )sin ( 2 ⁄ ).