We deposited thin films of thiophene/phenylene co-oligomers (TPCOs) onto poly(tetrafluoroethylene) (PTFE) layers that were friction-transferred on substrates. These films were composed of aligned molecules in such a way that their polarizations of emissions and absorbances were larger along the drawing direction than those perpendicular to that direction. Organic field-effect transistors (OFETs) fabricated with these films indicated large mobilities, when the drawing direction of PTFE was parallel to the channel length direction. The friction-transfer technique forms the TPCO films that indicate the anisotropic optical and electronic properties.