Monodomain liquid crystal elastomers (MLCEs), exhibiting a light-induced dynamic exchange reaction (DER) and light-triggered actuation abilities, were prepared using dispersed multiwalled carbon nanotubes (MWCNTs) and allyl sulfide linkages incorporated in the MLCE matrix. MWCNTs were dispersed in the MLCE matrix using a newly synthesized dispersant, poly(4-cyanobiphenyl-4′-oxyundecylacrylate-co-pyrene methyl acrylate); this dispersant exhibited amphiphilic properties of π–π interactions with the MWCNT fillers (attributed to the pyrene moieties) and miscibility with the MLCE matrix (attributed to the cyanobiphenyl mesogenic moieties). A low amount of well-dispersed MWCNTs (≤0.05 wt%) in the MLCE matrix induced excellent photothermal effects under near-infrared (NIR) light irradiation, leading to considerable reversible contraction/extension actuation (∼40 % change in length). The bilayer film comprising the MLCE and PLCE (PLCE: polydomain LCE) composite films bonded via DER without glue exhibited excellent bending actuation under NIR light irradiation and was configured into several actuators such as a flower-shaped actuator, a weightlifter, a circular rolling band, an oscillator mimicking a hummingbird, and a casting catapult. Therefore, this novel MLCE/CNT composite film enhances the design ability for the arbitrary shaping and functionalization of NIR light-triggerable LCE actuators, which can be applied to several interesting soft robots.
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