We describe the generation of aligned carbon nanotube bundles and films by pyrolysis of solid organic precursors (for example 2-amino-4,6-dichloro-s-triazine, s-triaminotriazine) at 950-1050 °C over laser-patterned thin metal (Fe, Co, Ni) films, deposited on silica substrates. Scanning electron microscopy (SEM) and atomic force microscopy (AFM) studies reveal that surface roughness of the laser-etched catalytic substrates plays a key role in achieving control of nanotube growth. We believe that, during the etching process, the energised (ablated) metal clusters condense and recrystallise evenly, possibly as the metal oxide, within the edges or surface of the eroded regions. During pyrolysis these catalytic particles, embedded in the silica substrates, are responsible for carbon agglomeration and subsequent tube axial growth, suggesting that nanotube alignment strongly depends upon the etching conditions (for example laser power, pulse duration, and focal distance). The pyrolysed products (usually nanotubes or nanofibres) were characterised by SEM, high-resolution transmission electron microscopy (HRTEM), electron energy loss spectroscopy (EELS) and energy dispersive X-ray spectroscopy (EDX). Samples containing only small amounts of amorphous carbon and other carbonaceous particles are notably absent. We observe that the degree of graphitisation is dependent upon the catalyst and the organic precursor. Interestingly, a nitrogen content <=7% was detected within the nanofibres, which exhibit corrugated graphite-like morphologies. This pyrolytic method may be used to advantage in generating aligned heteroatomic nanostructures such as BxCyNz systems.