It is demonstrated that combined rotation and multiple-pulse spectroscopy (CRAMPS) based on MSHOT-3 homonuclear multiple-pulse decoupling represents a powerful method for determination of 1H chemical shielding anisotropies from polycrystalline powders. By virtue of high-order dipolar decoupling, large spectral width, resonance offset stability, and the absence of artifacts fromtilted-axis precession, MSHOT-3-based CRAMPS enables straightforward sampling of high-quality spectra. Comparison with explicit calculations, taking the effect of the multiple-pulse sequence into account, shows that the spectra may be simulated and iteratively fitted using standard software for the calculation of magic-angle spinning spectra influenced by chemical shielding anisotropy with the shielding interaction reduced by the scaling factor of the MSHOT-3 decoupling sequence. The method is demonstrated by experimental determination of 1H chemical shielding anisotropies for adipic acid, Ca(OH)2, malonic acid, and KHSO4. The data are compared with those determined previously from single-crystal NMR studies. Copyright 1998 Academic Press.