Single-crystal diamond films grown over a large area may open up a new field of solid-states physics and industry, because diamond has several advantageous properties such as high thermal conductivity, hardness and wide bandgap semiconducting characteristics. These advantages are most effectively obtained in the single crystalline phase. The highly oriented or heteroepitaxial growth of diamond is one of the most promising ways of obtaining single crystalline films. Of various substrates, heteroepitaxial growth on silicon (Si) or silicon carbide (SiC) has received much attention [8.1–8], because perfect and large single crystals can be provided in Si, and the development of large single-crystal SiC and heteroepitaxial SiC films on Si has advanced rapidly in recent years. However, highly oriented or heteroepitaxial diamond growth has also been realized on other materials, such as near noble metals, to exhibit the unique qualities of diamond with respect to nucleation and growth.