Aiming at gathering further information to evaluate the recently proposed1,2 mechanism of the salt effect in aqueous polymer solutions, experimental vapor−liquid equilibria (VLE), liquid−liquid equilibria (LLE), and volumetric-compressibility measurements were carried out for several polymer−amino acid aqueous systems. The constant water activity lines (obtained through the isopiestic method at 298.15 K) of aqueous polypropylene glycol 400 (PPG400) + alanine or glycine systems, which form aqueous biphasic systems (salting-out effect), have a concave and convex slope, respectively, in the one-phase and two-phase regions. However, all the investigated polyethylene glycols (PEG400, PEG2000, PEG6000, and PEG10000) do not form aqueous biphasic systems with alanine or glycine (salting-in effect) and their constant water activity lines have a convex slope. In the second part of this work, the apparent molar volume and isentropic compressibility of transfer of alanine and glycine from water to aqueous solutions of PEG200, PEG2000, PEG10000, and PPG400 were studied at different temperatures. The third part of this work is concerned with the determination of LLE phase diagrams for several ternary polymer−amino acid aqueous systems containing polymers PPG400 and PPG725 and amino acids alanine, glycine, serine, and proline at different temperatures. On the basis of the obtained cloud point values of aqueous solutions of PPG725 in the absence and presence of various amino acids, it was found that all the investigated amino acids have a salting-out effect on PPG725 in aqueous solutions and entropy is the driving force for biphasic formation.