Electrical devices for very-high frequency (VHF, 0.03 -- 0.3 GHz) and ultra-high frequency (UHF, 0.3 -- 3.0 GHz) are commonly used for communications. However, the wavelengths, lambda, of these frequency bands correspond to lengths between 10 and 0.1 m, resulting in prohibitively large devices. Materials with an index of refraction, n, greater than 1 can be used to effectively shrink these devices by a factor of 1/ n. In this thesis, magnetodielectric materials (MDM), where n ≥1, have been made to be used in additive manufacturing processes with strict particle size requirements and were developed using various methods, such as polyol reduction and conventional ceramic solid state processing. These materials were characterized using x-ray diffraction (XRD), scanning and transmission electron microscopy (SEM and TEM), vibrating sample magnetometry (VSM), to determine their crystalline, physical, and direct current (DC) magnetization properties. The techniques used to synthesize the MDM yielded particles that were chemically similar, but had drastically different physical properties which heavily influences their high-frequency electromagnetic properties. These materials were then uniformly dispersed into a non-conducting medium, such as a low-electrical loss polymer or resin, and formed into composite samples with variable volumetric loading. These composite samples were measured using several techniques to characterize the frequency-dependent electromagnetic (EM) properties, such as relative permeability, relative permittivity, and their respective losses. Finite element method (FEM) simulations were performed using these MDM-composites to design a spiral antenna to be used at approximately 585 MHz.
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