A N.M.R. study of diamagnetic salts and CoCl2in pure water and in 10 : 1 mole ratio aqueous mixtures of acetone, N,N-dimethylformamide, dimethylsulphoxide, dioxane, ethanol, methanol and N-methylformamide, has been carried out. Water chemical shift displacements indicate that this component extensively solvates most cations. These displacements are correlated with ion charge, entropy, size, and with the water concentration. Evidence for solvation by the organic component was provided by the water results, AlCl3solution studies, and paramagnetic studies. In the AlCl3solutions, in the DMF, DMSO, and NMF-H2O solvent mixtures, separate N.M.R. signals were observed for bulk and complexed organic solvent.