With the ubiquity of electronic devices, finding ways to improve quality or fabrication methods of components is an important area of study. This dissertation looks at two sets of materials that may be used to address this need. The first is a series of disordered perovskites of the form Nd⅔--xLi3 xTiO3. These materials are notable for the way the lithium becomes spontaneously patterned during synthesis into square planar regions, the dimensions of which are only dependent upon the initial concentration of lithium. Through the use of point-charge calculations, the paramagnetic and first-order quadrupole interaction tensors for each of the 28 unique lithium sites of the x = 0.083 concentration were calculated and used to accurately simulate the experimental spectra. From this, it was observed that the 28 crystallographically distinct sites present in that particular concentration could be grouped into three sets based on the principal values of the paramagnetic interaction tensors. Qualitative analysis of spectra from the other concentrations suggests that this grouping holds for other concentrations, with only the relative number of sites in each group changing. Additionally, jump dynamics were incorporated into the simulations of one of the sites in order to explain the broadening that occurs at lower temperatures. The second study included in this dissertation is focused on lithium in a pair of high-dielectric microwave ceramics, Ca(Li1/3Nb 2/3)O3 and (Ca2/3La1/3)(Li1/3 Nb2/3)O3. Experimental results are reported for the temperature-dependence of both the spin-lattice relaxation rate and the isotropic chemical shift for each material. For both samples, the isotropic shift was linear with temperature, with the isotropic shift of Ca(Li 1/3Nb2/3)O3 having a stronger temperature dependence (3.53 Hz·K-1 compared to 2.65 Hz·K -1). The spin-lattice relaxation rates of both samples follow an Arrhenius relationship with temperature, with Ca(Li1/3Nb 2/3)O3 sample having an activation energy of 5.08 kJ · (mol · K)-1 and (Ca2/3La1/3)(Li 1/3Nb2/3)O3 having an activation energy of 2.21kJ · (mol · K)-1. In addition to the lithium study, there were also spectra acquired that observed the niobium nucleus in each material, which has a noticeably more complex spectrum. For the (Ca2/3 La1/3)(Li1/3Nb2/3)O3 sample, a double-quantum satellite-transition magic angle spinning pulse sequence was used to determine the isotropic chemical shift as well as the quadrupole product of each of the five resolved sites.