Solid-state potassium-39 NMR spectra of two potassium complexes of crown-ether-based organic ligands (1-KI and 2) have been acquired at 11.75 and 21.1 T and interpreted to provide information on the K-39 quadrupolar and chemical shift tensors. The analyses reveal a large potassium chemical shift tensor span of 75 20 ppm for 1-KI. This appears to be the first such measurement for potassium in I an organic complex, thereby suggesting the utility of potassium chemical shift tensors for characterizing organic and biomolecular K+ binding environments. Compound 2 exhibits a cation-g interaction between K+ and a phenyl group, and therefore, the 39K NMR tensors obtained for this compound must be partly representative of this interaction. Analyses of potassium-39 spin-rotation data for gaseous (KF)-K-39-F-19 and (KCl)-K-39-Cl-31 available from molecular beam experiments performed by Cederberg and co-workers reveal the largest potassium CS tensor spans known to date, 84.39 and 141 ppm, respectively. Collectively, the results obtained highlight the potential of ultrahigh-field potassium-39 solid-state NMR spectroscopy and, in particular, the wide range of the anisotropy of the potassium CS tensor when organic and diatomic systems are considered.