The cloud-point pressure of poly(t-butylaminoethyl methacrylate) [Poly(TBAEMA)] in various solvents such as supercritical carbon dioxide (CO2), dimethyl ether (DME) and t-butylaminoethyl methacrylate (TBAEMA) was measured to maximum pressure and temperature of 218.79 MPa and 452.9 K, respectively. The phase behavior for the Poly(TBAEMA)+CO2+TBAEMA mixture was investigated according to the various contribution factors, such as pressure, temperature and concentration with TBAEMA mass fraction of 9.9 wt%, 10.4 wt%, 14.9 wt%, 24.4 wt% and 35.2 wt%. The cloud point curves for the Poly(TBAEMA)+CO2+DME (15.6–78.7 wt%) systems show the variation of the (p, T) curve from upper critical solution temperature (UCST) region to lower critical solution temperature (LCST) region as DME concentration increases. The experimental data for the CO2+TBAEMA system were reported at the broad temperature range of 313.2 K to 393.2 K and the pressure range of 3.70 MPa to 20.62 MPa. The CO2+TBAEMA binary system shows the type-I phase behavior with a continuous critical mixture curve, and is correlated by Peng-Robinson equation of state with the critical properties for TBAEMA obtained by Joback and Lyderson group contribution method.