Diamond-like nanocomposite (DLN) thin films, comprising the networks of a-C:H and a-Si:O were deposited on pyrex glass or silicon substrate using gas precursors (e.g., hexamethyldisilane, hexamethyldisiloxane, hexamethyldisilazane, or their different combinations) mixed with argon gas, by plasma enhanced chemical vapor deposition technique. Surface morphology of DLN films was analyzed by atomic force microscopy. High-resolution transmission electron microscopic result shows that the films contain nanoparticles within the amorphous structure. Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, and x-ray photoelectron spectroscopy (XPS) were used to determine the structural change within the DLN films. The hardness and friction coefficient of the films were measured by nanoindentation and scratch test techniques, respectively. FTIR and XPS studies show the presence of C-C, C-H, Si-C, and Si-H bonds in the a-C:H and a-Si:O networks. Using Raman spectroscopy, we also found that the hardness of the DLN films varies with the intensity ratio ID/IG. Finally, we observed that the DLN films has a better performance compared to DLC, when it comes to properties like high hardness, high modulus of elasticity, low surface roughness and low friction coefficient. These characteristics are the critical components in microelectromechanical systems (MEMS) and emerging nanoelectromechanical systems (NEMS). © 2010 American Institute of Physics.