Atomic layer deposition (ALD) of metal oxides (MO) was used to modify the properties of nanographite (NG) films produced by direct current plasma–enhanced chemical vapor deposition technique. NG films consist of a few layers of graphene flakes (nanowalls) and nanoscrolls homogeneously distributed over a silicon substrate with a predominantly vertical orientation of graphene sheets to the substrate surface. and layers, with thicknesses in the range of 50 to 250 nm, were deposited on NG films by ALD. The obtained NG-MO composite materials were characterized by scanning electron microscopy, energy dispersive x-ray analysis, and Raman spectroscopy. It was found that ALD forms a uniform coating on graphene flakes, while on the surface of needle-like nanoscrolls it forms spherical nanoparticles. Field emission properties of the films were measured in a flat vacuum diode configuration. Analysis based on obtained current–voltage characteristics and electrostatic calculations show that emission from NG- films is determined by the nanoscrolls protruding from the coverage. The layers with thicknesses of almost do not affect the overall field emission characteristics of the films. At the same time, these layers are able to stabilize the NG films’ surface and can lead to an improvement of the NG cold cathode performance in vacuum electronics.