Medical tablet forming ability of microcrystalline cellulose (MCC) was investigated in relation to the mobility of water molecules in MCC particles, For this purpose, the spin-lattice relaxation time T-1 of water in the system was measured by H-1-NMR. Over a wide range of water contents (0.02 less than or equal to H2O/cellulose (g/g) less than or equal to 1.79), two different T-1 (T-1,T-l and T-1,T-s) values were observed for water in each MCC sample, Below the equilibrium water content, water having these two different T-1 values exchange with each other in an MCC particle reaching an equilibrium state within a given time scale (equilibrium constant K). The T-1,T-l, T-1,T-s and K values for water in MCC, estimated at the equilibrium water content, showed fairly good correlations with the hardness of the tablets made by the MCC samples, Sample with a shorter T-1, or larger K tended to have a stronger tablet forming ability, In the spin-spin relaxation time T-2 measurements for protons in an MCC/D2O system, two T-2 components originating from the glassy cellulose solid (T-2,T-G) and the swelling region (T-2,T-J) were observed. It was found that the mole fraction x(L) of protons with T-2,T-L in the system exhibits a clear linear correlation with K, From these results, a structural model for the distribution of water in MCC particles was propoed by taking the surface of each microfibril and the disordered region within the microfibril into consideration.