Aligned multi-walled carbon nanotubes (30-130 mum long, 10-200 nm outer diameter) have been prepared in high yield by pyrolysing homogeneously dispersed aerosols generated from benzene/ferrocene solutions, at 800 degreesC or 950 degreesC, using a compressed gas (Ar) driven atomiser. Scanning electron microscopy (SEM) and TEM studies reveal the presence of carpet-like flakes containing high yields of partly filled carbon nanotubes. X-ray diffraction confirms the presence of graphite-like structures, alpha -Fe and Fe3C (cementite). Nanotube and filling yields were found to be temperature and ferrocene concentration dependent. The preparative method opens up new avenues for nanotube synthesis based upon hydrocarbon/catalyst solutions.