Resist-free antireflective (AR) nanostructured films are directly fabricated on polycarbonate (PC) film using thermal-nanoimprint lithography (T-NIL) and the moth-eye shape of AR nanostructure is elaborately optimized with different oxygen reactive ion etching conditions. Anodic aluminum oxide (AAO) templates are directly used as master molds of T-NIL for preparation of AR nanostructures on PC film without an additional T-NIL resist. AR nanostructures are well arranged with a period of about 200 nm and diameter of about 150 nm, which corresponds to those of the AAO template mold. The moth-eye AR nanostructures exhibit the average reflectance of 2% in wavelength range from 400 to 800 nm. From the results, highly enhanced AR properties with simple direct imprinting on PC film demonstrate the potential for panel application in the field of flat display, touch screen, and solar cells.