A simple, yet innovative method is developed for fabricating high aspect-ratio polymer nanostructures (aspect ratio > 20) on a solid substrate by sequential application of molding and drawing of a thin polymer film. In this method, a thin polymer film is prepared by spin coating on a rigid or flexible substrate and the temperature is raised above the polymer’s glass transition while in conformal contact with a poly(urethane acrylate) (PUA) mold having nano-cavities. Consequently, capillary forces induced deformation of the polymer melt into the void spaces of the mold and the filled nanostructure was further elongated upon removal of the mold due to tailored adhesive force at the mold/polymer interface. The optimum value of the work of adhesion at the mold/polymer interface ranged from 0.9 to 1.1 times that at the substrate/polymer interface. Below or above this range, a simple molding or detachment occurred, corresponding to earlier findings.