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Abstract The fabrication of pressure sensitive adhesives (PSAs) using liquid crystal elastomers (LCEs), which are known for their excellent dissipation properties, is explored in this work. The adhesive properties of the PSAs are evaluated using the 180° peeling test at various conditions. The performance of the LCE adhesives is found to show significant rate and temperature dependence. When the adhesion energy is plotted against the rate, LCE shows an anomalously large power law exponent (n≈ 1.17) compared to existing PSAs (n≈ 0.1–0.6). The unusual rate sensitivity is hypothesized to originate from the synergy of soft elasticity and non‐linear viscoelasticity. The adhesive properties at various rates and temperatures are correlated to the results from dynamic mechanical analysis. Moreover, the large strain stiffening behavior of LCE under uniaxial tension reveals the distinctive advantages offered by LCE as adhesives. Time‐temperature superposition is used to obtain a master curve of adhesion energy that spans rates beyond typical experimental limits. The extreme rate dependence and the large strain stiffening of LCE yield a new category of adhesives that possess special properties, such as reversible adhesion and impact resistance, unlike traditional adhesives. 

Fibers capable of generating axial contraction are commonly seen in nature and engineering applications. Despite the broad applications of fiber actuators, it is still very challenging to fabricate fiber actuators with combined large actuation strain, fast response speed, and high power density. Here, we report the fabrication of a liquid crystal elastomer (LCE) microfiber actuators using a facile electrospinning technique. Owing to the extremely small size of the LCE microfibers, they can generate large actuation strain (~60 percent) with a fast response speed (<0.2 second) and a high power density (400 watts per kilogram), resulting from the nematic-isotropic phase transition of liquid crystal mesogens. Moreover, no performance degradation is detected in the LCE microfibers after 10⁶cycles of loading and unloading with the maximum strain of 20 percent at high temperature (90 degree Celsius). The small diameter of the LCE microfiber also results in a self-oscillatory behavior in a steady temperature field. In addition, with a polydopamine coating layer, the actuation of the electrospun LCE microfiber can be precisely and remotely controlled by a near-infrared laser through photothermal effect. Using the electrospun LCE microfiber actuator, we have successfully constructed a microtweezer, a microrobot, and a light-powered microfluidic pump.