Polytwistane is an intriguing hydrocarbon nanorod that has not been experimentally realized to date. To facilitate its identification in complex reaction mixtures, the ¹H and ¹³C nuclear magnetic resonance (NMR) spectra of idealized polytwistane were calculated using two distinct quantum chemical approaches. In addition, the NMR spectra of related hydrocarbon nanorods were determined. On the basis of these data, we speculate whether polytwistane and its congeners correspond to a crystalline one-dimensional sp³ carbon nanomaterial formed by high-pressure solid-state polymerization of benzene.