The polyurethane (PU) copolymer was grafted with either 3-dimethylaminopropanol as a basic pendant group or 4-hydroxylphenylacetic acid as an acidic pendant group. The two types of PU were mixed in solution to form ion-pairing between acidic and basic pendant groups. The structural change after grafting and ion-pairing was followed by acid-base titration, infrared spectra, differential scanning calorimetry, and absolute viscosity. The tensile stress can be raised as much as 70 % by the control of the ion-pairing ratio of acidic and basic PUs. Shape recovery was over 80 % and reproducible for four test cycles. The minor control of tensile properties of PU was possible through the ion-pairing method.