Water proton relaxation measurements obtained from model cellular systems composed of red blood cell (RBC) ghosts are presented. The purpose of the investigation was to evaluate hypotheses concerning the possible sources of multiple exponential components in similar relaxation measurements made on tissue. Both laboratory frame transverse and longitudinal relaxation rates, as well as rotating frame relaxation rates, were measured in preparations of RBC ghosts and “extracellular fluid” that were, (a) uniformly mixed or (b) compartmentalized by layering, as the concentration of serum albumin was varied in the “extracellular fluid.” The data show that although transmembrane exchange is too fast to give rise to multiexponential relaxation, multiple components can result from compartmentalization at the level of the cellular organization and do not necessarily require different tissue types. In addition, the data clearly demonstrate the importance of protein adsorption to cellular membranes as a determinant of the concentration of freely mobile solute protein molecules in tissue fluids. © 1991 Academic Press, Inc. Copyright © 1991 Wiley‐Liss, Inc., A Wiley Company