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A variety of benefits motivate the development of epitaxial metals, among which include the ability to design fully integrated layer structures where metallic films and nanostructures can be embedded into the cores of optoelectronic devices. Applications include high-performance tunnel-junctions, epitaxial transparent Ohmic contacts, photomixer material, and thermoelectrics. Additionally, the integration of metallic nanostructures and films into optoelectronic devices has shown potential for improving device performance and functionality through sub-wavelength confinement of plasmonic modes and enhancement of light/matter interactions. The rare-earth monopnictide (RE-V) material system can be integrated epitaxially with conventional zincblende III-V substrates under normal growth conditions, resulting in high-quality, thermodynamically stable interfaces. The RE-V semimetals span a range of optical, electrical, and structural properties, making them ideal for integration into III-V-based optoelectronic devices and applications. In this dissertation, high-quality epitaxial LuAs, LaAs and La(x)Lu(1-x)As films and nanostructures were grown and characterized for their structural, electrical, optical, and plasmonic properties. Through a sweep of alloy film compositions of the RE-V alloy material La(x)Lu(1-x)As, the ability to produce tunable epitaxial metals was demonstrated, with a range of peak transmission spectra from near- to mid-infrared wavelengths, plasmonic response in the mid-infrared, moderate resistivity, and lattice-matching potential to many relevant III-V substrates. Additionally, there is a great deal of interest in developing techniques to produce optoelectronic devices that are not restricted by substrate lattice constant. Many epitaxial approaches have been tried, with moderate success; however, growing low defect-density heteroepitaxial materials with differing crystal structures and highly-mismatched lattice parameters is extremely challenging, and such structures suffer from poor thermal properties and reliability issues. A general approach is needed for thin metamorphic buffer layers with minimal threading dislocations that simultaneously have low thermal resistance for effective heat-sinking and device reliability. An investigation was conducted into the use of RE-V nanostructure superlattices towards the reduction of dislocation density in highly-mismatched III-V systems. / text