Abstract
The current development of soft shape-memory materials often results in materials that are typically limited to the synthesis of thin-walled specimens and usually rely on complex, low-yield manufacturing techniques to fabricate macro-sized, solid three-dimensional objects. However, such geometrical limitations and slow production rates can significantly hinder their practical implementation. In this work, we demonstrate a shape-memory composite material that can be effortlessly molded into arbitrary shapes or sizes. The composite material is made from main-chain liquid crystal elastomer (MC-LCE) microparticles dispersed in a silicone polymer matrix. Shape-programmability is achieved via low-temperature induced glassiness and hardening of MC-LCE inclusions, which effectively freezes-in any mechanically instilled deformations. Once thermally reset, the composite returns to its initial shape and can be shape-programmed again. Magnetically aligning MC-LCE microparticles prior to curing allows the shape-programmed artefacts to be additionally thermomechanically functionalized. Therefore, our material enables efficient morphing among the virgin, thermally-programmed, and thermomechanically-controlled shapes.