Liquid−liquid equilibrium data were obtained for aqueous two-phase system (ATPS) composed of [poly(ethylene oxide) (PEO1500), poly(propylene oxide) (PPO425), poly(ethylene oxide) 11 −poly(propylene oxide) 17 −poly(ethylene oxide) 11 (L35), or poly(propylene oxide) 8 −poly(ethylene oxide) 22 −poly(propylene oxide) 8 (10R5)] + ammonium thiosulfate + water, at 283.2, 298.2, and 313.2 K. The consistencies of the all tie-line experimental compositions were improved by applying the Othmer− Tobias and Bancroft equations, resulting in linear correlation coefficients (R 2 ) ≥ 0.95. For all the ATPS, an increase in the temperature resulted in increases in the biphasic region and the tie-line slope, indicating that the phase separation process was entropically driven. Among the macromolecules studied, PPO425 produced the largest biphasic region, due to its greater hydrophobicity, followed by L35 ≈ 10R5 > PEO1500.