Monoselective, Rio(SE), biselective, Rio(i,j), and nonselective proton spin-lattice relaxation rates have been measured for dilute solutions of gramicidin S in dimethyl sulfoxide and used to evaluate cross-relaxation rates (sigma ij = Rio(i,j)-Rio(SE)) and Fi ratios (Fi = Ri(NS)/Rio(SE)). The cross-relaxation parameters, sigma, and Fi ratios measured for backbone gramicidin S protons predict that the same correlation time, tau c = 1.2 X 10(-9)s, modulates all the dipolar proton-proton interactions and that these interactions represent the main source for the proton spin-lattice relaxation process. The larger relaxation rates for amide versus alpha-protons of the backbone are attributed to dipolar relaxation between 14N and its directly bonded protons and is an approximate measure of the extent of this. The intrabackbone proton-proton distances, evaluated from sigma values, were consistent with the antiparallel beta-plated sheet/beta II'-turn conformation previously proposed for gramicidin S in solution.