Diamond is a very interesting material with a wide range of properties, making it highly applicable, for example, in power electronics, chemo- and biosensors, tools’ coatings, and heaters. Due to the high demand for this innovative material based on the properties it is already expected to have, it is important to obtain homogeneous diamond layers for specific applications. Doping is often chosen to modify the properties of layers. However, there is an alternative way to achieve this goal and it is shown in this publication. The presented research results reveal that the change in methanol content during the Hot Filament Chemical Vapour Deposition (HF CVD) process is a sufficient factor to tune the properties of deposited layers. This was confirmed by analysing the properties of the obtained layers, which were determined using Raman spectroscopy, scanning electron microscopy (SEM), X-ray diffraction (XRD), and an atomic force microscope (AFM), and the results were correlated with those of X-ray photoelectron spectroscopy (XPS). The results showed that the increasing of the concentration of methanol resulted in a slight decrease in the sp3 phase content. At the same time, the concentration of the -H, -OH, and =O groups increased with the increasing of the methanol concentration. This affirmed that by changing the content of methanol, it is possible to obtain layers with different properties.