Single crystal, type IIa natural diamond substrates have been implanted with 4 MeV carbon ions to doses ranging from 0.5–130×1016 cm-2. The accumulation of implantation damage is studied by Raman and RBS/channeling. Similar effects are observed for crystals of , , and  orientation but with different rates of damage accumulation. With increasing implantation damage, the triply degenerate Raman mode at 1332 cm-1 broadens and shifts down to around 1300 cm-1. This corresponds to a peak in the one-phonon density of states as predicted for Raman from an amorphous sp 3 network. There is no evidence for the existence of sp 2 carbon in the implanted area. Additional non-graphite Raman peaks appear at 1451, 1494, and 1635 cm-1. At the higher doses, the 1332 cm-1 Raman mode is no longer observed; however, RBS/channeling still shows the surface region to be crystalline and it is possible to grow high quality homoepitaxial diamond films on these substrates.