In this paper, nanoimprint lithography was utilized to transfer a nano-pattern (NP) onto a homeotropic polyimide (PI) surface for use in liquid crystal displays (LCDs). The nano-patterned silicon mold was fabricated by laser interference lithography. A NP PI layer acted as the homeotropic alignment layer to easily and uniformly align the liquid crystal (LC) molecules. A NP LC cell with a NP PI layer was successfully operated as a vertical aligned LCD, and its performance was evaluated. The threshold voltage and response time of the NP LC cell were 2.472 V and 22.7 ms, respectively. In addition, the NP LC cell was characterized by a high thermal budget. Therefore, the competitive performance of the NP LC cell could allow new approaches to replace the conventional rubbing process in display technology.