Diamond-like carbon (DLC) flakes were produced using a dual-frequency method: microwave/radiofrequency plasma-assisted chemical vapour deposition (MW/RF PACVD) with the use of methane or its mixture with gases such as hydrogen, argon, oxygen or nitrogen. Their modification was performed using a planetary ball mill with and without a fluid: deionised water or methanol. Changes occurring in the morphology of flake surfaces were presented in pictures taken using a scanning electron microscope (SEM). Their composition and chemical structure were analysed using Raman spectroscopy and X-ray photoelectron spectroscopy (XPS). The presented research results show that it is possible to control the size of flakes and their chemical structure. An increase in the C-C sp 3 bond content in produced carbon-based materials is only possible by modifying DLC flakes during their production process by introducing oxygen or argon into the working chamber together with the carbon-carrying gas. In the processes of mechanical DLC flake modification, it is necessary to add fluid to limit the occurrence of graphitisation processes. The research conducted shows that methanol is best used for this purpose as its use results in a decrease in the percentage of C-C sp 3 bonds as compared to the materials, before milling, of only 1.7%. A frequent problem both in the production of DLC flakes and during their mechanical modification is the introduction of additional elements into their structure. Admixing electrode materials from the plasma-chemical device (iron) or grinding beads (zirconium) to DLC flakes was observed in our studies. These processes can be limited by the appropriate selection of production conditions or by mechanical modifications.