Solid-state nuclear magnetic resonance (SSNMR) is a powerful tool for probing structural differences in local environments for both crystalline and amorphous materials. As a local probe of structure, SSNMR can be a highly effective characterization tool, because long-range order (often required for diffraction methods) is not needed. Consequently, there is broad applicability of NMR across chemical, biological and materials science fields, characterizing diverse systems ranging from battery anodes, to biological solids, to zeolites. The most familiar NMR methods have focused on nuclear spin -½ (I=1/2) systems, such as 1 H and C; however, a majority of NMR-active isotopes are quadrupolar, with I > ½, which can yield exquisite details about the interaction between the nuclear spin and its surrounding ground state electron density produced by the EFGs . Even with the revolutionary demonstration of new NMR pulse-sequence methods for quadrupolar species in the 1990's (resulting in highly resolved spectra) , quadrupolar SSNMR is still often plagued by complicated lineshapes that can overlap and become difficult to elucidate for structural features. Hence, "NMR crystallography" --using a combination of SSNMR, X-ray diffraction and quantum mechanical simulation methods to determine the components of tensors --relates atomic positions to the corresponding spectra. --have been transformative to interpretation of SSNMR of quadrupolar species.