Predicting and controlling the properties of amphiphile aggregate mixtures require understanding the arrangements and dynamics of the constituent molecules. To explore these topics, we study molecular arrangements and dynamics in alkyl ethoxylate nonionic surfactant micelles by combining NMR relaxation measurements with large-scale atomistic molecular dynamics simulations. We calculate parameters that determine relaxation rates directly from simulated trajectories, without introducing specific functional forms to describe the dynamics. NMR relaxation rates, which depend on relative motions of interacting atom pairs, are influenced by wide distributions of dynamic time scales. We find that relative motions of neighboring atom pairs are rapid and liquidlike but are subject to structural constraints imposed by micelle morphology. Relative motions of distant atom pairs are slower than nearby atom pairs because changes in distances and angles are smaller when the moving atoms are further apart. Large numbers of atom pairs undergoing these slow relative motions contribute to predominantly negative cross-relaxation rates. For spherical micelles, but not for cylindrical micelles, cross-relaxation rates are positive only for surfactant tail atoms connected to the hydrophilic headgroup. This effect is related to the lower packing density of these atoms at the hydrophilic-hydrophobic boundary in spherical vs cylindrical arrangements, with correspondingly rapid and less constrained motion of atoms at the boundary.