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Abstract The electrically‐directed, isothermal response of liquid crystal elastomers (LCEs) to an applied electric field is a compelling approach to realize spatially tailorable, sequence‐controllable, and high‐frequency deformation. The electromechanical response is facilitated by coating aligned LCEs with compliant electrodes. Upon application of an electric field, the electrodes attract and generate Maxwell stress. The directional difference in moduli for aligned LCEs produces directional deformation of the material and does not require mechanical bias or framing. Here, LCEs prepared from a newly reported thiol‐ene reaction are explored as DEAs with improved mechanical and dielectric properties. This report details that incorporating a difunctional liquid crystalline monomer composed of allyl ether functional groups reduces Young's modulus, increases the dielectric constant, and improves cyclic recovery compared to an analogous LCE prepared by thiol‐ene polymerization. Electrically‐induced, isothermal deformation of as much as 30% strain is reported. The facile chemistry and enhanced electromechanical response reported here may enable the functional integration of LCEs in applications such as robotics.