Nanohole-structured single-crystalline Pt nanosheets have been synthesized by the borohydride reduction of Na2PtCl6 confined to the lyotropic liquid crystals (LLCs) of polyoxyethylene (20) sorbitan monooleate (Tween 80) with or without nonaethylene-glycol (C12EO9). The Pt nanosheets of around 410 nm in central thickness and up to 500 nm or above in diameter have a number of hexagonal-shaped nanoholes similar to 1.8 nm wide. High-resolution electron microscope images of the nanosheets showed atomic fringes with a spacing of 0.22 nm indicating that the nanosheets are crystallographically continuous through the nanoholed and non-holed areas. The inner-angle distributions for the hexagonal nanoholes indicate that the six sides of the nanoholes are walled with each two Pt (111), Pt (1(1) over bar 1) and Pt (010) planes. The formation mechanism of nanoholed Pt nanosheets is discussed on the basis of structural and compositional data for the resulting solids and their precursory LLCs, with the aid of similar nanohole growth observed for a Tween 80 free but oleic acid-incorporated system. It is also demonstrated that the nanoholed Pt nanostructures loaded on carbon exhibit fairly high electrocatalytic activity for oxygen reduction reaction and a high performance as a cathode material for polymer-electrolyte fuel cells, along with their extremely high thermostability revealed through the effect of electron-irradiation.