Increasing strengths of liquid crystalline polymers while minimizing anisotropy via topological rearrangement assisted bi-directional stretching of reversibly interlocked macromolecular networks

• Strengthening crosslinked liquid crystalline epoxy while minimizing anisotropy. • Reversibly interlocked polymers networks can be biaxially stretched at solid-state. • The biaxially oriented interlocked networks containing mesogens can self-heal. To prepare oriented crosslinked liquid crystalline polymers (LCPs) while preventing the unwanted anisotropy, the authors fabricated interlocked networks from liquid crystalline epoxy and amorphous polyurethane, which are crosslinked by reversible Diels-Alder (DA) bonds and Schiff base, respectively. By making use of dynamicity of the reversible bonds as well as relative mobility of the parent networks of the interlocked networks, the material is subjected to stepwise solid-state bi-directional drawing. Owing to the directional alignment of the mesogens and molecular chains and the increased crosslinking density during stretching caused by the networks reshuffling, the strengths of the material in orthogonal directions are simultaneously improved and gradually converged to the values comparable to the reported highest level of unidirectionally orientated crosslinked LCPs. Furthermore, the biaxially oriented interlocked networks have inherited the intrinsic self-healing capability from the included reversible bonds. The proposed method is easy to use and expected to contribute to the practical applications of crosslinked LCPs, which is becoming more and more important in modern microelectronics and communication technology.