The fabrication of a single polymer
network that exhibits a good
reversible two-way shape memory effect (2W-SME), can be formed into
arbitrarily complex three-dimensional (3D) shapes, and is recyclable
remains a challenge. Herein, we design and fabricate poly(thiourethane)
(PTU) networks with an excellent thermadapt reversible 2W-SME, arbitrary
reconfigurability, and good recyclability via the synergistic effects
of multiple dynamic covalent bonds (i.e., ester, urethane, and thiourethane
bonds). The PTU samples with good mechanical performance simultaneously
demonstrate a maximum tensile stress of 29.7 ± 1.1 MPa and a
high strain of 474.8 ± 7.5%. In addition, the fraction of reversible
strain of the PTU with 20 wt % hard segment reaches 22.4% during the
reversible 2W-SME, where the fraction of reversible strain is enhanced
by self-nucleated crystallization of the PTU. A sample with arbitrarily
complex permanent 3D shapes can be realized via the solid-state plasticity,
and that sample also exhibits excellent reversible 2W-SME. A smart
light-responsive actuator with a double control switch is fabricated
using a reversible two-way shape memory PTU/MXene film. In addition,
the PTU networks are de-cross-linked by alcohol solvolysis, enabling
the recovery of monomers and the realization of recyclability. Therefore,
the present study involving the design and fabrication of a PTU network
for potential applications in intelligent actuators and multifunctional
shape-shifting devices provides a new strategy for the development
of thermadapt reversible two-way shape memory polymers.