Divisions, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831 USA.Laser interactions with materials have unique advantages to explore the rapid synthesis, processing, and in situ characterization of high quality and novel nanoparticles, nanotubes and nanowires. For example, laser vaporization of solids into background gases provides a wide range of processing conditions for the formation of nanomaterials by both catalyst-free and catalyst-assisted growth processes. Laser interactions with the growing nanomaterials provide remote in situ characterization of their size, structure, and composition with unprecedented temporal resolution. In this article, laser interactions involved in the synthesis of primarily carbon nanostructures are reviewed, including the catalyst-free synthesis of single-walled carbon nanohorns and quantum dots, to the catalyst-assisted growth of single and multi-walled carbon nanotubes.