Gold nanoparticles offer the possibility of creating metamaterials; however, such nanoparticles are not particularly stable. Conversely, liquid crystals offer the possibility of creating self-organizing and self-assembling materials, which can be designed to be relatively stable. Potentially, combining these two concepts could provide materials that can be induced to assemble in a controlled way and that would have unique optical properties. This article describes some of the groundwork made in the preparation of stable liquid-crystalline metamaterials and the investigation of their structures and physical properties. In particular, spherically substituted materials are found to be deformed into tactoids with anisotropic properties, most notably their dielectric anisotropies.