Diamond-like carbon (DLC) films have been deposited by radio frequency plasma enhanced chemical vapour deposition (rf-PECVD) with different Ar-CH4 mixtures. Nanocrystalline diamond films have been deposited by microwave plasma-enhanced chemical vapour deposition (MPCVD), using Ar-H2-CH4 mixtures. X-ray photoelectron spectroscopy (XPS) and nanotribological investigation (by scanning force microscopy) have been used to compare the mechanical properties and structures of these films. Highly orientated and non-orientated microcrystalline diamond films and MPCVD-produced amorphous carbon have also been studied by way of comparison. The diamond films exhibit a linear relationship between roughness and the coefficient of friction. The DLC and amorphous carbon have higher friction coefficients than the best performing diamond film, but may more easily be deposited as smooth coating. Possible applications for these various carbon-based films include microelectromechanical components, for which smooth, hard coatings are required.