The pulsed-gradient, spin-echo technique has been used to study self-diffusion of protons in several colloidal systems in order to examine the usefulness of that technique in determining the extent to which the free movement of molecules in these systems is restricted by the colloidal structures present. The pulsed-gradient experiment is preferred to the steady-gradient experiment because it affords better definition and control over the time during which diffusion is observed. Diffusion times between 1 sec and 10-3 sec have been used. One artificial system of thin liquid layers, three different kinds of plant cells, and one emulsion have been studied. Clear indications of restricted diffusion are found in all the systems. When fitted to theoretical expressions derived for such behavior, the data yielded a description of each system, as seen by the diffusing molecules, adequately in agreement with the known structure and properties. Critiera for recognizing and analyzing restricted diffusion are discussed. Necessary conditions for the successful study of restricted diffusion are also discussed.