The work presents the results of the scanning electron microscopy (SEM) and Raman spectrometry studies of carbonaceous nanostructures containing nickel nanocrystallites. The films were obtained using a two-step method. In the first phase the Physical Vapour Deposition (PVD) method was applied, whereas in the second Chemical Vapour Deposition (CVD) method was used. The paper presents results for samples with various Ni content obtained with different parameters of the two-phase technological process. The research confirms that the thin films obtained by PVD method contain Ni nanocrystallites distributed in a carbonaceous matrix. The matrix is composed of various carbon allotropes (amorphous carbon, graphite, fullerene). The thin films made by CVD method make a matrix when multiwalled, carbonaceous nanotubes are obtained. Depending on the technological process parameters of each phase, we obtain multiwall nanotubes with a various degree of defects.