Magnetization transfer and NMR relaxation rates were measured for water protons in two types of polymer gels developed for radiation dosimetry with MRI in order to quantify the contributions of different relaxation processes to the radiation response in such gels. Measurements included the rate of magnetization transfer between proton pools and the ratio of the sizes of exchanging pools, R1 and R2. A model of relaxation in irradiated gels is presented to explain their properties. The model incorporates three proton pools: free water, macromolecular and interfacial. Two pools are insufficient to model the data. In these systems, radiation-induced polymerization appears to increase the size of a solid-like macromolecular proton pool but does not affect the rate constant of magnetization transfer per proton from macromolecular protons to the free water protons. The relation between R1 and the pool size ratio is consistent with free water exchanging with a macromolecular pool with an R1 of approximately 8 Hz. In addition, the rate of magnetization transfer is not limited by the rate of chemical exchange between the free water and the interfacial protons, and magnetization transfer most probably occurs via labile proton exchange rather than via bound water molecules.