© 2016 Inderscience Enterprises Ltd. The aim of the present paper concerns investigations of cobaltcontaining nano-materials by means of nuclear magnetic resonance (NMR) technique. A comparison is made among the 59Co NMR spectra of nanocomposites synthesised under different conditions and using different precursors. All studied nano-composite samples exhibit the hcp structure-type of á-Co and the existence of canted spins in the near-surface layers in spite of both the different type of stabilising matrixes and the proportion of Co-metal in the systems. The spectra analysis shows that the NMR method can be used for operative control and can lead to selection of the optimal conditions to design composite materials with desirable properties.