At sufficiently high temperatures PLD deposited TaC films can be grown epitaxially on 4H-SiC (0001) substrates; at lower temperatures the films recrystallize and ball up forming a large number of pinholes. The growth temperature for epitaxy was found to be 1000°C, and it was facilitated by the epitaxial growth of a thin (2 nm) transition layer of hexagonal Ta 2C. High temperature annealing produced changes in the surface morphology, caused grain growth, and created pin holes through a recrystallization process in the films deposited at the lower temperatures, while the films deposited at the higher temperatures remained virtually unchanged. Using TEM it is shown that the (0001) basal planes of the hexagonal 4H-SiC and Ta2C phases are aligned, and they were also parallel to the (111) plane in the cubic TaC with the [101̄] cubic direction being parallel to the hexagonal [2110̄] hexagonal direction. The Ta2C interlayer most likely is formed because its lattice parameter in the basel plane (3.103 Å) is intermediate between that of the 4H-SiC (3.08 Å) and the TaC (3.150 Å). Given that Al.5Ga.5N is lattice matched to TaC, it could be an excellent substrate for the growth of GaN/AlGaN heterostructures. © (2009) Trans Tech Publications, Switzerland.