Single-crystal time-of-flight neutron diffraction has provided atomic resolution of H atoms of H2O molecules and hydroxyl groups, as well as Li cations in the uranyl peroxide nanocluster U-60. Solid-state magic-angle-spinning nuclear magnetic resonance (MAS NMR) spectroscopy was used to confirm the dynamics of these constituents, revealing the transportation of Li atoms and H2O through cluster walls. H atoms of hydroxyl units that are located on the cluster surface are involved in the transfer of H2O and Li cations from inside to outside and vice versa. This exchange occurs as a concerted motion and happens rapidly even in the solid state. As a consequence of its large size and open hexagonal pores, U-center dot(60) exchanges Li cations more rapidly compared to other uranyl nanoclusters.