Abstract
In this study, we present an approach to enhance the thermo-mechanical performance of liquid crystal elastomers (LCEs) by inducing chain entanglements through mechanical kneading. This process creates a network of highly entangled polymer chains, significantly improving the mechanical properties of LCEs, over a wide range of strain rates and temperatures. Mechanical kneading also improves the actuation performance, resulting in higher actuation stresses, greater contraction, and increased tolerance to self-rupture at elevated temperatures. Chain entanglements can also serve as a crucial enabler for the fabrication of monodomain LCEs. Using entanglements as the initial cross-linking step provides sufficient elasticity to LCEs, enabling the synthesis of aligned LCEs. This work demonstrates the benefits of chain entanglements, offering a pathway for the design and fabrication of high-performance LCE-based actuators for advanced applications.