Recently, geometrically structured nanomaterials have received great attention due to their unique physical and chemical properties, which originate from the geometric variation in such materials. Indeed, the use of various geometrically structured nanomaterials has been actively reported in enhanced‐performance devices in a wide range of applications. Recent significant progress in the development of geometrically structured nanomaterials and associated devices is summarized. First, a brief introduction of advanced nanofabrication methods that enable the fabrication of various geometrically structured nanomaterials is given, and then the performance enhancements achieved in devices utilizing these nanomaterials, namely, i) physical and gas nanosensors, ii) nanoelectromechanical devices, and iii) nanosieves are described. For the device applications, a systematic summary of their structures, working mechanisms, fabrication methods, and output performance is provided. Particular focus is given to how device performance can be enhanced through the geometric structures of the nanomaterials. Finally, perspectives on the development of novel nanomaterial structures and associated devices are presented.