The generation of nanostructures by initial layer deposition and plasma etching offers a simple and cost‐effective method for imparting broadband anti‐reflection properties to polymer optics. In this study, we have investigated the possibility of controlling the structure growth on the cycloolefin polymer Zeonex®. It has been found that the geometry of the emerging nanostructures can be adjusted from “island‐like,” through “sponge‐like,” to “pinholes” merely by changing the thickness of the initial layer before the etching step. However, not all structure types provided a satisfactory transmittance enhancement. Only when the initial layer thickness and the etching time were matched in such a way that a certain material/air filling factor range and a sufficient structure depth were obtained could an outstanding anti‐reflection effect be realized.