Abstract Proton spin-lattice relaxation rates (R 1 values) have been measured at 400 MHz for a series of substituted aromatic compounds to determine the steric effects of ortho substituents on the R 1 values of the methyl groups. These values have been interpreted on the basis of differences in the barriers to methyl group rotation caused by the substituent, resulting in changes in the contributions from the dipolar and the spin-rotation relaxation ...