We report on some scanning probe microscopy observations of the morphology of both metallic and diamond-like carbon thin films formed using a vacuum are plasma deposition method with ion energy control. The metal films investigated were Cu, Mo, Ta and W, and the diamond-like carbon films were hydrogen-free and with sp(3):sp(2) fraction (i.e. diamond content) up to as high as 85%; film thicknesses were 300-2000 Angstrom. The microscopy was done using both atomic force and scanning tunneling modes. We found that all of the films were smooth to the one or two atomic-layer level. The atomic-level smoothness of the films and the ability to modify their microstructure makes them attractive for a number of fundamental and technological applications.