Integration
of multiple types of dynamic linkages into one polymer
network is challenging and not well understood especially in the design
and fabrication of dynamic polymer nanocomposites (DPNs). In this
contribution, we present facile methods for synthesizing flexible,
healable, conductive, and recyclable thermoresponsive DPNs using three
dynamic chemistries playing distinct roles. Dynamic hydrogen bonds
account for material flexibility and recycling character. Thiol-Michael
exchange accounts for thermoresponsive properties. Diels–Alder
reaction leads to covalent bonding between polymer matrix and nanocomposite.
Overall, the presence of multiple types of orthogonal dynamic bonds
provided a solution to the trade-off between enhanced mechanical performance
and material elongation in DPNs. Efficient reinforcement was achieved
using <1 wt % multiwalled carbon nanotubes as nanocomposite. Resulting
DPNs showed excellent healability with over 3 MPa increase in stress
compared to unreinforced materials. Due to multiple responsive dynamic
linkages, >90% stress–relaxation was observed with self-healing
achieved within 1 h of healing time. Increased mechanical strength,
electrical conductivity, and reprocessability were achieved all while
maintaining material flexibility and extensibility, hence highlighting
the strong promise of these DPNs in the rapidly growing fields of
flexible compliant electrodes and strain sensors.