The electro-optical (EO) characteristics of twisted nematic (TN) cells based on poly(vinylidene fluoride-trifluoroethylene) [PVDF-TrFE] films have been studied, including the effects of rubbing and ion-beam (IB) irradiation alignment methods and the use of different PVDF-TrFE precursor concentrations during film fabrication. Homogeneously and uniformly aligned liquid crystal (LC) molecules were obtained on PVDF-TrFE films prepared using both 3 wt% and 5 wt% precursor concentrations. TN cells based upon IB-irradiated PVDF-TrFE films operated normally, but those based upon rubbed PVDF-TrFE films operated with superior performance.