AbstractA scalable fabrication route combining colloidal lithography and nanoskiving is reported for generating free‐standing asymmetric metal nanostructures of crescent‐shaped gold nanowires and rows of opposing crescents with and without nanogaps. Strong localized surface plasmon resonances and propagating surface plasmon polaritons are excited at the sharp tips of the crescent and in the sub‐10 nm nanogaps. High‐order resonance modes are excited due to the coupling between the resonances in the tips and gaps. The Raman signals are greatly enhanced due to the strong electric fields. In addition, the optical responses and electric field distributions can be controlled by the polarization of the incident light. The strong electric field enhancement coupled with facile, scalable fabrication make crescent‐shaped nanostructures promising in nonlinear optics, optical trapping, and surface‐enhanced spectroscopy.