The objective of this dissertation is to develop amorphous metal thin films (AMTFs) for two-terminal electrical device and nanolaminate applications. Two AMTFs, ZrCuAlNi and TiAl, are investigated in both two-terminal electrical device and nanolaminate applications. Material properties including composition, atomic order, surface morphology, surface potential, and electrical resistivity are explored. Application of AMTFs as electrodes in tunneling MIM diodes leverages the ultra-smooth AMTF surface morphology which results from the amorphous atomic order of AMTFs. Analysis methodologies using tunneling MIM diode I-V characteristics are described. A methodology used to estimate potential barrier heights is applied to tunneling MIM diode with differing lower electrode material, upper electrode material and upper electrode deposition technique. A second methodology used to estimate relative tunneling MIM diode insulator thickness is also presented. The presented I-V characteristic analysis methodologies illustrate that tunneling MIM diodes fabricated with AMTF lower electrodes possess tunable I-V characteristics. Nanolaminates are layered materials fabricated with alternating dissimilar thin-film layers. The flexibility of AMTF nanolaminates is illustrated through the presentation of amorphous metal/oxide nanolaminates fabricated with differing AMTFs and aqueous solution deposited oxides. TEM and XPS depth profile analysis of realized nanolaminates are presented. The optical dielectric response of ZrCuAlNi/aluminum phosphate oxide (AlPO) and TiAl/AlPO nanolaminates are evaluated through polarized reflectance measurements and effective medium theory. The optical dielectric response of the nanolaminates differ from the optical dielectric response of the component layers. ZrCuAlNi/AlPO and TiAl/AlPO nanolaminates therefore satisfy the definition of metamaterials. / Graduation date: 2012 / Access restricted to the OSU Community at author's request from May 9, 2012 - May 9, 2013