Proton magnetic resonance pH NMR) has been used to determine the second moment (M2) of the line shape, solid echo decay, and dipolar (Tld), rotating frame (Tlp) and spin-lattice (Tt) relaxation times of unaltered, crystallite-enriched, and gelled-reprecipitated samples of cotton and filter paper cellulose.For all samples, the measured M2 was within 30% of that for the rigid lattice, indicating that cellulose microfibrils are almost rigid on the NMR time scale of 10"5 s. Measurements of 7\ as a function of frequency indicated the presence of a low amplitude but important motion occurring in cellulose at about 10-15 MHz which may be methylol group reorientation. Measurements of Tld, Tlp, and the solid echo decay revealed the presence of two types of domains which we assign to crystalline and paracrystalline cellulose. Crystallite-enriched cellulose contained material of only one domain type. Cellulose of reduced crystallinity (gelled-reprecipitated) contained a corresponding increase in the domain we assigned to paracrystalline cellulose. Our results are in agreement with a model in which the crystalline cellulose domains consist of rigid crystalline microfibrils with cross-sectional widths of 100-400 Á and the paracrystalline cellulose domains consist of smaller elementary fibrils with lower packing density.