A single‐step process of radio frequency‐catalytic chemical vapor deposition (RF‐cCVD) was used for the synthesis of pelletized ceramic carbon nanotube (CNT) composites. The surface resistance of the insulating magnesium oxide (MgO) was found to drop dramatically as the result of the graphitic nanostructures formed within the ceramic matrix after the catalytic process. It was found that the electrical properties of the ceramic CNT composites were highly dependent on the concentration of the loading metal that was responsible for the formation of different carbon species on the MgO pellet. Hall effect measurements of ceramic single‐walled CNT composites indicated an n‐type electrical behavior with high carrier densities of around 2.5 × 1020/cm3 and electrical mobilities of 1.1 cm2/V s. The process is shown to be useful for generating ceramic CNT devices that may be used for a variety of applications.