Abstract1H high‐resolution NMR spectra of polycrystalline alkali trihydrogen selenites were measured at 270 MHz using the combination of a multiple‐pulse sequence and magic angle sample spinning. Good resolution of the separate1H NMR lines belonging to different hydrogen bonds in these crystals was obtained. Correlations between the measured average values of the chemical shift tensor and the parameters characterizing hydrogen bond [R(O…O) andR(H…O)] distances and the deuteron quadrupolar coupling constante2qQ/hare presented. These correlations are found to be linear, with high correlation coefficients for the ordered protons. The possibilities of designating disordered protons on finding large deviations from the correlations for ordered protons are di