We use multi-dimensional solid-state NMR methods, particularly a mix of quantitative, dipolar-mediated, and multiple-quantum NMR experiments, to understand solids at atomic and sub-nanometer length scales (e.g., through-bond connectivities and through-space distances). Often, we are interested in elucidating ionic and electronic charge storage mechanisms in battery electrodes, or characterizing defects, disorder, or amorphous components critical to material properties but otherwise challenging to measure.