Polyurethane (PU) was graft polymerized with poly(acrylic acid) (PA) to form a PA-grafted PU (UA) series, and a control PU (C) series containing free PA was also prepared for comparison. The grafted PA could be ionized, and an ionized PA-grafted PU (IUA) series was separately prepared. The spectroscopic, thermal, tensile, shape memory, low-temperature flexibility, and water permeability properties of the polymer series were compared. With an increase in the PA content, the T (m) did not change, but Delta H (m) decreased for the UA, IUA, and C series. The T (g) did not significantly change with the increase in PA content for the UA, IUA, and C series. The tensile strengths of the UA and IUA series sharply increased with the PA content, whereas that of the C series did not. The breaking strain of the UA, IUA, and C series remained the same with the increase in PA content. The shape recovery and shape retention of the PU-PA series remained high after four repeated tests. Finally, the IUA series PU demonstrated better low-temperature flexibility and water compatibility than the unmodified PU.