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The development of fibrous actuators with diverse actuation modes is expected to accelerate progress in active textiles, robotics, wearable electronics, and haptics. Despite the advances in responsive polymer-based actuating fibers, the available actuation modes are limited by the exclusive reliance of current technologies on thermotropic contraction along the fiber axis. To address this gap, the present study describes a reversible and spontaneous thermotropic elongation (~30%) in liquid crystal elastomer fibers produced via ultraviolet-assisted melt spinning. This elongation arises from the orthogonal alignment of smectogenic mesogens relative to the fiber axis, which contrasts the parallel alignment typically observed in nematic liquid crystal elastomer fibers and is achieved through mesophase control during extrusion. The fibers exhibiting thermotropic elongation enable active textiles increase pore size in response to temperature increase. The integration of contracting and elongating fibers within a single textile enables spatially distinct actuation, paving the way for innovations in smart clothing and fiber/textile actuators. 

Abstract Materials that undergo reversible changes in form typically require top‐down processing to program the microstructure of the material. As a result, it is difficult to program microscale, 3D shape‐morphing materials that undergo non‐uniaxial deformations. Here, a simple bottom‐up fabrication approach to prepare bending microactuators is described. Spontaneous self‐assembly of liquid crystal (LC) monomers with controlled chirality within 3D micromold results in a change in molecular orientation across thickness of the microstructure. As a result, heating induces bending in these microactuators. The concentration of chiral dopant is varied to adjust the chirality of the monomer mixture. Liquid crystal elastomer (LCE) microactuators doped with 0.05 wt% of chiral dopant produce needle‐shaped actuators that bend from flat to an angle of 27.2 ± 11.3° at 180 °C. Higher concentrations of chiral dopant lead to actuators with reduced bending, and lower concentrations of chiral dopant lead to actuators with poorly controlled bending. Asymmetric molecular alignment inside 3D structure is confirmed by sectioning actuators. Arrays of microactuators that all bend in the same direction can be fabricated if symmetry of geometry of the microstructure is broken. It is envisioned that the new platform to synthesize microstructures can further be applied in soft robotics and biomedical devices.