We have investigated the formation of various multilayer thin films by the laser physical vapor deposition technique. A multi stage target holder was constructed to perform all process steps in-situ; target/substrate cleaning, deposition, and annealing. The laser physical vapor deposition technique offers many advantages over conventional physical vapor techniques, such as, lower substrate temperature, microstructural control, and very low contamination levels. Film thickness can be controlled from near atomic to micron dimensions. A layer-by-layer (two dimensional) growth can be achieved, resulting in nonequilibrium structures. The films were analyzed using cross-section and high resolution transmission electron microscopy (TEM). The significant reduction in substrate temperature for the formation of high quality multilayer and epitaxial films opens up many new areas of applications requiring reduced thermal-budget processing.