A premixed flame burner system was utilised to synthesise carbon nanotubes (CNTs). The morphologies of highly-graphitic carbon nanotubes were characterised by using transmission electron microscopy (TEM) and X-ray powder diffraction (XRD). The XRD analysis shows the spectrum of a typical CNT, while TEM imaging shows the physical structure of the carbon nanotubes. CNTs were grown effectively on a Ni-contained substrate in an elevated temperature environment. The flame synthesised CNTs were of high crystalline, multi-wall structure, and contained relatively less impurities and amorphous carbon. The CNT intershell spacing values quantified using TEM and XRD are 0.317 nm and 0.344 nm respectively. CNTs produced from flame synthesis are based on the tip-growth model and vapor-liquid-solid (VLS) mechanism.