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Garnet-like structures containing lithium are of interest for applications in lithium ion batteries because of their inherent lithium ion conductivity and stability against chemical reaction with Li. Here, a series of materials, with parent composition LaLi0.5Fe0.2O2.09, are synthesized using solid-state chemistry, and characterized, in terms of their structure, using a combination of powder X-ray diffraction (PXRD), 7Li, and 139La solid-state NMR, which reveal disorder on the Li and Fe sites in the lattice. The 7Li spectra comprise a set of peaks that are distinguished based on their T1 relaxation properties, as a diamagnetic set and a paramagnetic set of peaks. The 139La spectra include two La environments, one well-defined, with a CQ of 56 MHz ± 1 MHz and asymmetry parameter, η of 0.05 ± 0.05, and a second, which experiences a range of local environments, because of the Li/Fe substitution, and has a CQ of 29 MHz ± 2 MHz, and η of 0.6 ± 0.1. The dynamics within the materials were characterized using imp...