This research consists of an experimental and theoretical investigation of grain growth in polycrystalline films on single crystal substrates. Reflected high energy and transmission electron diffraction, transmission electron microscopy, and thin film X-ray texture analysis are employed to characterize the film grain size and orientation. Metal-on-metal, metal-on-mica, and metal-on-alkali halide model systems are the principal materials under study. Experimental results on grain growth are compared to predictions from computer simulations and analytical theories. A primary goal is to determine the film/substrate interface energy as a function of relative film/substrate orientation by experimental methods and compare these results with atomistic computer simulations.