The pyrolysis of a block copolymer thin film, the free surface of which was in contact with air or a capping layer of SiO2, produced four carbon nanostructures. Thin films of a diblock copolymer having perpendicularly oriented lamellar nanodomains served as carbon and nitrogen precursors. Before pyrolysis, the lamellar nanodomains were cross-linked with UV irradiation under nitrogen gas (UVIN). Without a capping layer, pyrolysis caused a structural transformation from lamellar nanodomains to short carbon nano wires or to dropletlike nanocarbons in a row via Rayleigh instability, depending on the duration of pyrolysis. When capped with a layer of SiO2 followed by pyrolysis, the lamellar nanodomains were converted to pod-like, spaghetti-like, or long worm-like carbon nanostructures. These carbon nanostructures were driven by controlling the surface or interface tension and the residual yield of solid carbonaceous species.