Poly(diisopropylaminoethyl methacrylate) (PDPA) is a pH- and thermally responsive water-soluble polymer. This study deepens the understanding of its phase separation behavior upon heating. Phase separation upon heating was investigated in salt solutions of varying pH and ionic strength. The effect of the counterion on the phase transition upon heating is clearly demonstrated for chloride-, phosphate-, and citrate-anions. Phase separation did not occur in pure water. The buffer solutions exhibited similar cloud points, but phase separation occurred in different pH ranges and with different mechanisms. The solution behavior of a block copolymer comprising poly(dimethylaminoethyl methacrylate) (PDMAEMA) and PDPA was investigated. Since the PDMAEMA and PDPA blocks phase separate within different pH- and temperature ranges, the block copolymer forms micelle-like structures at high temperature or pH.