Pulse laser ablation and subsequent laser nanostructuring at room temperature has been employed to produce nanostructured Ni on SiO₂/Si substrates for catalytic growth of carbon nanotubes. The resultant nanostructured surface is seen to consist of nanometer sized hemispherical droplets whose mean diameter is controlled by the initial metal thickness, which in turn is readily controlled by the number of laser pulses. Vertically aligned multiwall carbon nanotube mats were then grown using conventional plasma enhanced chemical vapor deposition. We show that within a single processing technique it is possible to produce the initial metal-on-oxide thin film to a chosen thickness but also to be able to alter the morphology of the film to desired specifications at low macroscopic temperatures using the laser parameters. The influence of the underlying oxide is also explored to explain the mechanism of nanostructuring of the Ni catalyst.