LAUSR

Soft robots are susceptible to premature failure from physical damages incurred within dynamic environments. To address this, we report an elastomer with high toughness, room temperature self‐healing, and strong adhesiveness, allowing both prevention of damages and recovery for soft robotics. By functionalizing polyurethane with hierarchical hydrogen bonds from ureido‐4[1H]‐pyrimidinone (UPy) and carboxyl groups, high toughness (74.85 MJ m−3), tensile strength (9.44 MPa), and strain (2340%) can be achieved. Furthermore, solvent‐assisted self‐healing at room temperature enables retention of high toughness (41.74 MJ m−3), tensile strength (5.57 MPa), and strain (1865%) within only 12 h. The elastomer possesses a high dielectric constant (≈9) that favors its utilization as a self‐healing dielectric elastomer actuator (DEA) for soft robotics. Displaying high area strains of ≈31.4% and ≈19.3% after mechanical and electrical self‐healing, respectively, the best performing self‐healable DEA is achieved. With abundant hydrogen bonds, high adhesive strength without additional curing or heating is also realized. Having both actuation and adhesive properties, a “stick‐on” strategy for the assembly of robust soft robots is realized, allowing soft robotic components to be easily reassembled or replaced upon severe damage. This study highlights the potential of soft robots with extreme ruggedness for different operating conditions.