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Establishing structure–property correlations is of paramount importance to materials research. The ability to selectively detect observable magnetization from transitions between quantized spin states of nuclei makes nuclear magnetic resonance (NMR) spectroscopy a powerful probe to characterize solids at the atomic level. In this article, we review recent advances in NMR techniques in six areas: spectral resolution, sensitivity, atomic correlations, ion dynamics, materials imaging, and hardware innovation. In particular, we focus on the applications of these techniques to materials research. Specific examples are given following the general introduction of each topic and technique to illustrate how they are applied. In conclusion, we suggest future directions for advanced solid-state NMR spectroscopy in interdisciplinary research. Expected final online publication date for the Annual Review of Materials Research, Volume 50 is July 1, 2020. Please see http://www.annualreviews.org/page/journal/pubdates for revised estimates. 

Abstract The performance of all‐solid‐state batteries (ASSBs) relies on the Li⁺transport and stability characteristics of solid electrolytes (SEs). Li₃PS₄is notable for its stability against lithium metal, yet its ionic conductivity remains a limiting factor. This study leverages local structural disorder via O substitution to achieve an ionic conductivity of 1.38 mS cm⁻¹with an activation energy of 0.34 eV for Li₃PS_4−xO_x(x = 0.31). Optimal O substitution transforms Li⁺transport from 2D to 3D pathways with increased ion mobility. Li₃PS_3.69O_0.31exhibits improvements in the critical current density and stability against Li metal and retains its electrochemical stability window compared with Li₃PS₄. The practical implementation of Li₃PS_3.69O_0.31in ASSBs half‐cells, particularly when coupled with TiS₂as the cathode active material, demonstrates substantially enhanced capacity and rate performance. This work elucidates the utility of introducing local structural disorder to ameliorate SE properties and highlights the benefits of strategically combining the inherent strengths of sulfides and oxides via creating oxysulfide SEs.