Nuclear magnetic relaxation measurements of water in gels made of crosslinked dextran or polyacrylamide (water content, 30-60 wt%) were camed out using broad-line proton-pulsed NMR. Both T, and T2 values showed inflection against pore size, i.e., the size of the compartment made by crosslinks of the polymer gels. Tz (or T , ) values obtained for gels with compartments smaller than the critical size remained low within the range of the water content used in this experiment. Those values of gels with larger compartments, on the other hand, became higher with increasing size. When the size of the compartment was larger than the critical size, T I and Tz values also became higher with increasing water content. The inflection point can be considered to correspond to the critical compartment size below which the motion of compartmentalized water in gels is more or less restricted. When the compartment is small, however, not only the effect of the molecular motion of water but also that of the proton exchange between compartmentalized water and gel matrix or hydration water should be taken into consideration for the interpretation of the short relaxation times observed, especially by Tz. The results obtained in this investigation might provide useful information in the explanation and evaluation of the relaxation values in tissue.