Low-molar-mass organic compounds can form oriented crystal fibers on various substrates by a simple casting technique. A dilute solution of an aromatic organic compound, such as a tetrathiofulvalene derivative, an annulated aromatic such as tetracene, or a perylene diimid, is cast on a substrate, and the solvent is allowed to evaporate while rolling a glass bar over the substrate. Because the crystal formation takes place at the solution edge, crystals grow in the roller direction. Optical microscopy, fluorescence microspectrometry, and scanning nearfield optical microscopy were used to characterize the resulting fibers and crystals. Casting on interdigitated electrodes enabled us to measure conductivity and field effect transistors in these oriented crystals.