Multinuclear spin-lattice relaxation rates, cross-relaxation rates and self-diffusion coefficient measurements are reported over wide ranges of temperature, pressure and concentration in undercooled aqueous solutions of tetraalkylammonium bromides. These dissolved organic cations with apolar surface groups provide model systems to investigate the effect of coulombic, hydrophobic and H-bond interactions upon the solvent and solute dynamics within the random, transient H-bond network of undercooled water.