A study was conducted to demonstrate a simple method for fabricating stopped high-aspect-ratio (AR) nanohairs of polyurethane acrylate (PUA) material that utilized replica molding and post-electron-beam irradiation. The method offered a facile route to prepare angled polymer nanohairs without multistep processes or surface treatment. It was demonstrated that the PUA material was molded into a geometry controlled and high-density nanochair surface with an AR of up to 10 without facing self-matting problem, due to its favorable mechanical properties. The as-formed hairy structures also allowed for structural transformation into directional and angled nanohairs, while maintaining better adhesion capability. The nanohair surface also showed significant unidirectional adhesion properties and a higher shear adhesion due to its structural similarity to natural gecko foot hairs.