In this paper, electctrohydrodynamic (EHD) printing was utilized to print polyimide (PI) materials for use in liquid crystal (LC) alignment layers in LC displays (LCDs). We produced the PI layer using the multi-jet mode of EHD printing. Homogeneous LC orientation was uniformly achieved on the EHD-printed PI layer, and a twisted nematic (TN) LC cell with an EHD-printed PI layer was created and compared with a conventional spin-coated PI-based TN LC cell. From the results, EHD printing has potential for use to print the PI layer in an LCD process. (C) 2012 The Electrochemical Society. [DOI: 10.1149/2.029206esl] All rights reserved.