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Wang, Yuchen; Dang, Alei; Zhang, Zhifeng; Yin, Rui; Gao, Yuchong; Feng, Liang; Yang, Shu (, Advanced Materials)Abstract Liquid crystal elastomers (LCEs) are of interest for applications such as soft robotics and shape‐morphing devices. Among the different actuation mechanisms, light offers advantages such as spatial and local control of actuation via the photothermal effect. However, the unwanted aggregation of the light‐absorbing nanoparticles in the LCE matrix will limit the photothermal response speed, actuation performance, and repeatability. Herein, a near‐infrared‐responsive LCE composite consisting of up to 0.20 wt% poly(ethylene glycol)‐modified gold nanorods (AuNRs) without apparent aggregation is demonstrated. The high Young's modulus, 20.3 MPa, and excellent photothermal performance render repeated and fast actuation of the films (actuation within 5 s and recovery in 2 s) when exposed to 800 nm light at an average output power of ≈1.0 W cm−2, while maintaining a large actuation strain (56%). Further, it is shown that the same sheet of AuNR/LCE film (100 µm thick) can be morphed into different shapes simply by varying the motifs of the photomasks.more » « less