Laser interactions have traditionally been at the center of nanomaterials science, providing highly nonequilibrium growth conditions to enable the synthesis of novel new nanoparticles, nanotubes, and nanowires with metastable phases. Simultaneously, lasers provide unique opportunities for the remote characterization of nanomaterial size, structure, and composition through tunable laser spectroscopy, scattering, and imaging. Pulsed lasers offer the opportunity, therefore, to supply the required energy and excitation to both control and understand the growth processes of nanomaterials, providing valuable views of the typically nonequilibrium growth kinetics and intermediates involved. Here we illustrate the key challenges and progress in laser interactions for the synthesis and in situ diagnostics of nanomaterials through recent examples involving primarily carbon nanomaterials, including the pulsed growth of carbon nanotubes and graphene.