Completely inorganic nanoscale clusters play an essential role in many aspects of inorganic chemistry, materials chemistry, and geochemistry. The underlying dynamic behavior of these species in solution defines how and why they make successful thin film precursors as well as exist naturally in the environment. There have been a limited number of previous solution studies involving inorganic nanoscale clusters due to the lack of spectroscopic handles and availability of analytical techniques. This dissertation outlines the available and appropriate characterization techniques needed for identifying and studying inorganic nanoscale species and then uses proton Nuclear Magnetic Resonance (1H-NMR) and Diffusion Ordered Spectroscopy (DOSY) to fully characterize the Ga13-xInx(µ3-OH)6(µ-OH)18(H2O)24(NO3)15 (0 ≤ x ≤ 6) cluster series in solution. This research lays a foundation for a multitude of future studies on the dynamic behavior of these species that was previously unachievable. This dissertation includes previously published and unpublished co-authored material.