A carbon/carbon composite was used as substrate for low-pressure diamond deposition. To enhanced diamond nucleation on carbon/carbon composites, a total of ten surface preparation methods have been investigated. These methods involved the use of atomic hydrogen etching, mechanical polishing, sonication, or coating. Diamond nucleation was found to occur on either the defects of the carbon/carbon composite substrates or diamond particulate left on the substrates. The defects were created primarily by atomic hydrogen etching during the coating process. Seeding with diamond powders was performed by dip coating, sonication, or spray-coating processes. It was found that these seeding processes resulted in excellent nucleation of diamond.