High-dielectric-constant (k) materials and electrical devices implementing the high-k materials are provided herein. According to some embodiments, an electrical device includes a substrate and a crystalline-oxide-containing composition. The crystalline-oxide-containing composition can be disposed on a surface of the substrate. Within the crystalline-oxide-containing composition, oxide anions can form at least one of a substantially linear orientation or a substantially planar orientation. A plurality of these substantially linear orientations of oxide anions or substantially planar orientations of oxide anions can be oriented substantially perpendicular or substantially normal to the surface of the substrate such that the oxide-containing composition has a dielectric constant greater than about 3.9 in a direction substantially normal to the surface of the substrate. Other embodiments are also claimed and described.