The (meta)stability of low water activity sodium hydroxide/aluminate (Na+OH-/Al(OH)4-) electrolytes dictates kinetics in the Bayer process for aluminum refining and high-level nuclear waste processing. We utilized quasi-elastic neutron scattering (QENS) and proton nuclear magnetic resonance spectroscopy (1H NMR) in extremely concentrated sodium aluminate solutions to investigate the picosecond (ps) to microsecond (ms) timescale motions of H-bearing species (Al(OH)4- monomers/clusters, OH- and H2O). In the QENS data, in contrast to typical liquids, no short-time translational diffusion was observed at 293 K, but two types of localized motions were found: (i) local backbone tumbling or a formation of large hydrated ion clusters on the order of 40-60 ps; and (ii) much slower, complex, and collective dynamics of the ensemble of H-bearing species on the order of 350-750 ps. Variable temperature, pulsed field gradient, diffusion-ordered 1H NMR was used to determine the ensemble translational motion along with relaxometry to calculate rotational correlation coefficients. The ensemble rotational correlation times were on the order of 184-300 ps from 1H NMR, which is consistent with the timescale of the QENS components. Complementary molecular dynamics simulation of NaOH solutions exhibit extensive ion networks potentially responsible for the observed dynamical coupling of water with the motion of large hydrated ion clusters. Understanding these collective motions will aid in predicting the behavior of complex solutions during aluminum production and during nuclear waste processing.