Vertically‐Aligned Fringe‐Field Switching (VA‐FFS) liquid crystal (LC) mode is known for its intrinsic submillisecond fast response time due to existence of “self‐imposed boundaries” or “virtual walls”. In this paper, we investigate the difference between VA‐FFS LC mode employing LC materials with positive and negative dielectric anisotropy for both 2D and 3D electrode designs. We found that, in general, positive LC materials can provide faster response time whereas negative LC materials can provide higher transmission. In the case of 2D design, negative LC is found to have unexpected slow response times due to i) existence of a 2‐step switching process and ii) disappearance of virtual walls. By using 3D design, both ofthese problems for negative LC have been found to be improved. Due to its fast response time, VA‐FFS LC has been actively researchedfor VR/AR applications in recent years.