For practical deployment of carbon nanotubes, an understanding of their growth mechanism is required in order to obtain better control over their crystallinity, chirality and other structural properties. In this study, we focus on the influences of gas species on carbon nanotube synthesis using thermal chemical vapour deposition. The influence of methane, hydrogen, and helium gases was investigated from the viewpoint of gas chemistry in relation to the nanotube structural change, by varying the growth pressure, the gas-flow ratio and the growth temperature. Simple changes in the hydrogen gas concentration during different growth stages have been found to induce surprising changes to the nanotube formation. The structure of the tubular carbon growth changed from amorphous to graphitic as the growth temperature and the concentration of hydrogen in the initial periods of growth decreases. The excess hydrogen tends to give rise to poor crystalline carbon nanofibres but has the effect of increasing the yields. Hydrogen gas is typically used in reducing metal catalyst particles during the pre-treatment and the carbon nanotube growth periods. We show that while hydrogen species can improve yield, it can also result in the degradation of the nanotube's crystallinity. The use of hydrogen in the growth process is one of the key parameters for enhanced control of carbon nanotube/nanofibre growth and their resulting crystallinity.