Laser-based Synthesis of Nanomaterials with in situ Diagnostics  – Research opportunities and techniques for nanomaterials and thin-film synthesis utilizing in situ laser-based imaging and spectroscopy at the CNMS will be described. New windowed furnaces and chambers at CNMS permit laser-vaporization (LV), CVD, and PLD of novel nanomaterials and thin films to be explored and probed using tunable nanosecond-OPO laser probes, gated optical spectroscopy, and fast imaging. Examples of nanomaterials synthesis by LV, CVD, and PLD will be reviewed, including photoluminescent Si-nanoparticles, single-walled carbon nanotubes and nanohorns, and vertically aligned nanotube arrays.