High-resolution transmission electron microscopy ͑HRTEM͒ was used to characterize the cross-sectional and planar atomic structures and bonding states of highly tetrahedrally bonded amorphous carbon ͑ta-C͒ films, particularly concentrating on the surface layer and interface between substrate and pure ta-C film. A ''sandwich'' cross-sectional structure was found to be existing in ta-C grown from hyperthermal carbon species, and can be expressed as A/B/A layer-by-layer stacks. The interface ͑A͒ was shown to be very thick ͑ϳ40 nm͒, and consisted of sp 2 -bonded carbon domains and quasicontinuous two-dimensional layers. The initial pure carbon layer on silicon substrate exhibits relatively ordered atomic configuration, which can be attributed to the presence of graphitelike structure. The surface layer ͑A͒ was investigated in detail by using both cross-sectional and planar HRTEM observations. Results indicated a large number of ordered structure existed in the surface, in the manner of entangled ribbons that were identified to be sp 2 -bonded glassy carbon. The ordered sp 2 -bonded surface layer is proposed to form immediately while stopping deposition, i.e., the final stage of film growth, due to thermal spike-induced stress relaxation on surface. The interior film ͑B͒ is predicted to possess higher sp 3 -bond content than that measured by electron-energy-loss spectrum. In addition, slow positron annihilation, as well as a classical-trajectory calculation concerning the projected range R p and range straggling ⌬R p of carbon species implantation into silicon substrate, were conducted for further investigating and interpreting the observed atomic structures in surface, interior film, and interface. The fact that sp 2 -bonded surface and interface are present in a primarily sp 3 -bonded film gives a direct corroboration of subplantation model and compressive stress mechanism for sp 3 -bonded film growth from hyperthermal species.