Sulfur-33, because of its low natural abundance, spin of 3/2, and large quadrupole moment, has been a much neglected nucleus in nmr as well as in other branches of spectroscopy. The use of high rf power levels incident upon the sample, large modulation amplitudes, and signal averaging, however, permits nmr spectra with reasonable signal/noise ratios to be obtained. The present 33s nmr investigation was undertaken to explore the potential of the technique as a structure-determining tool. 33S chemical shifts and spectral line widths are presented for 12 materials. The range of chemical shifts is nearly 600 ppm, whereas spectral line widths vary from 0.2 to 16 g. The organic compounds investigated were carbon disulfide, dimethyl sulfoxide, ethyl disulfide, tetrahydrothiophene, thiophene, and three substituted thiophenes. The inorganic compounds examined included concentrated and dilute (10 n) sulfuric acid, aqueous sodium sulfide, and the sulfide anion in cubic zinc sulfide. The highest field resonances were observed for aqueous sodium sulfide and for s2-; the lowest field resonance was for 10 n sulfuric acid. The effects of high symmetry about sulfur and fast chemical exchange on 33s spectral line widths are discussed and illustrated. The 33s nmr results are compared with those of other nuclei in chemically similar compounds.