If the rapid reorientations of methyl groups in solids are the dominant relaxation mechanisms, it is theoretically found that the Zeeman system is dynamically coupled to the so-called rotational polarization system, resulting in a nonexponential Zeeman relaxation. Though this result has been confirmed experimentally, in many samples within measuring error an exponential Zeeman relaxation has been observed. In order to decide whether or not this is contradictory to the theory the degree of nonexponentiality has been further investigated in this paper. It is shown that the nonexponential character depends stronly on the following parameters: (i) the way in which the spin system is prepared for the observation of the Zeeman relaxation, (ii) the number of protons not belonging to the methyl groups, (iii) the relaxation due to the intermethyl dipolar interactions, and (iv) the temperature. It is found that under specific conditions the observed relaxation can become almost exponential. The corresponding time constant, however, can differ considerably from that predicted by the usual spin temperature theory. Therefore, the interpretation of the experiments with this theory can lead to incorrect values of the different parameters characterizing the relaxation process. The various results have been illustrated with experiments on polycrystalline samples of 2,6-dimethylphenol, methylcyanide, 2-methylpiperazine, and 1,4-dimethoxy-2,6-dimethylbenzene.