too small, the fibers will untwist before use; an excessive anchoring force will, on the other hand, prevent the fibers from moving and responding to external stimuli. [5][6][7][8] Therefore, the development of twist fibers in an untethered form will avoid the need for anchoring, simplify experimental design, and make various operations feasible. In practical applications, reversible rotational actuation is also important for twist fibers because it allows the fibers to respond to external stimuli repeatedly without the need to insert twists into the fibers each time before use. [9][10][11] In addition, high torque and rotational deformation are key factors in the operation of rotating microengines. The torque produced by the twist fibers must be sufficiently large to rotate objects. A large rotational deformation of the twist fibers is desirable for moving objects over a large distance in a wide range of applications. [12,13] So far, various materials have been utilized for untethered twist fibers that exhibit reversible rotational deformation upon stimuli. The actuation performance of these materials varies with the material. For example, twist fibers made from carbon materials or polymers can generate large rotational deformation of 588° mm −1 , but the generated specific torque reaches only 0.63 N m kg −1 . [9,10] To date, the construction of untethered twist fibers with reversible responsiveness, high torque, and large rotational deformation remains a challenge. A possible solution is the development of a material with high intrinsic deformation ratio and reversible responsiveness for fabricating twist fibers. [14] Among the various stimuli-responsive materials, liquid crystal elastomers (LCEs) have attracted increasing attention because of their dramatic and reversible stimuli-responsive deformation. [15][16][17][18][19][20][21][22][23] LCEs exhibit the two properties of high intrinsic deformation ratio and reliable reversibility which originate from the change in mesogenic alignment upon external stimuli. [24] These properties are important for improving the rotational performance of twist fibers. Here, we develop a template method based on a two-step cross-linking strategy to fabricate liquid crystal elastomer twist fibers (LCETFs). These untethered LCETFs can reversibly generate high torque and large rotational deformation. Fibers made from LCE have been widely exploited as actuators, [25][26][27][28] artificial muscles, [29][30][31][32] and soft robots. [33,34] In this work, we insert twists into LCE fibers Untethered twist fibers do not require end-anchoring structures to hold their twist orientation and offer simple designs and convenient operation. The reversible responsiveness of these fibers allows them to generate torque and rotational deformation continuously upon the application of external stimuli. The fibers therefore have potential in rotating microengines. In practical applications, high torque and rotational deformation are desirable to meet work capacity requirements. However, the simultan...