High-performance shape memory polymers with multifunctions are essential in sensors, wearable flexible electronics, artificial muscle actuators, and reversible morphing structures. In this work, a transparent and humidity-responsive shape memory polyurea featuring a high tensile strength (51 MPa), a high recovery stress (12 MPa) with an high energy output (0.98 J/g), and tolerance to extreme environments (retains great malleability at -196 °C) is prepared through constructing a bioinspired hard-soft nanophase structure and through hierarchical hydrogen bonding in the molecular network. The hard segment of a strong hydrogen bonding region is in charge of humidity-responsive behavior, and the soft segment of a weak bonding region provides the flexibility of the molecular chain. Furthermore, the periodicity of the phase-separated domains is 12 nm as characterized by small-angle X-ray scattering. The hydrogen bonding cross-linked network can be opened under the action of stress and re-bonded by heating, just like a zipper structure of reversible linking property. This unique molecular structure contributes to the humidity-responsive behavior of polyurea rolling up 160° in 20 s on the palm, as well as a high energy output lifting a 100 g weight exceeding 1631 times its own mass to 60 mm. The molecular structure of the hard-soft nanophase and the hierarchical hydrogen bonding offer an effective approach toward achieving a high-performance shape memory polymer with humidity-sensitive functions.
Keywords: energy output; high-performance shape memory polymers; humidity response; hydrogen bonding; polyurea.