Ionic polyurethanes with excellent properties have garnered significant attention in flexible wearables. However, it is still challenging to achieve ionic polyurethane ionotronics with both excellent mechanical properties and functionalization. Here, a series of hydroxypropyl viologen (HDPV) cationic-based supramolecular polyurethane with tunable strength (7.6-76.6 MPa), toughness (29.1-285.3 MJ m