We characterize a flexible self-assembled liquid crystal display (LCD) fabricated from a polyimide (PI) alignment layer with polydimethylsiloxane (PDMS) pixel walls. Ion-beam irradiation aligned liquid crystal molecules in the PI layer and bonded two flexible plastic substrates in a one-step assembly of the pixel walls. X-ray photoelectron spectroscopic analysis, Fourier transform infrared spectroscopy, and scanning electron microscopy provided chemical and physical evidence for the formation of stable chemical bonds between the PI layer and the PDMS pixel walls, in addition to the important maintenance of a uniform 6 mu m gap between the two substrates without the use of any epoxy resins or other polymers. Electro-optical performance of our flexible device was highly reliable, even under deformation conditions, and is comparable to that of conventional rigid glass substrate LCDs. (C) 2008 The Electrochemical Society. [DOI: 10.1149/1.2994632] All rights reserved.