Etching of natural diamonds by atomic hydrogen has been investigated on C(100), C(110), and C(111) single crystal surfaces. Infrared absorption spectroscopy and low-energy electron diffraction provide direct evidence for an etching anisotropy at 1100 K. The results indicate that, in the presence of atomic hydrogen, ͕111͖-oriented facet formation irreversibly occurs on both C(110) and C(100), whereas C(111) remains intact. The finding has important implications for chemical vapor deposition diamond synthesis and H-plasma surface polishing. [S0031-9007(97)03064-0]