The effect of lithium ion on the ordering of water in water-saturated nitrobenzene has been probed by H-2 NMR, diffusion ordered spectroscopy and neutron scattering. It was shown that increased water concentration in LiClO4/wet nitrobenzene results in the formation of a metastable solvatomer with mixed water and nitrobenzene character, Li-(W/NB)(+). This species is shown to decay over hours to two solvatomers, one dominated by nitrobenzene Li-(NB)(+) and the other dominated by water Li-(W)(+). To confirm the assignment of these solvation states, diffusion ordered deuterium NMR spectroscopy has been used to elucidate the hydrodynamic radii of these solvatomers. Neutron scattering yields vibrational spectroscopy information that shows how addition of lithium to the nitrobenzene/water system results in relatively slow self-organization of the water environment (hours).