Min‐Hui Li

Liquid crystal elastomers (LCEs) with promising applications in the field of actuators and soft robotics are reported. However, most of them are activated by external heating or light illumination. The examples of electroactive LCEs are still limited; moreover, they are monofunctional with one type of deformation (bending or contraction). Here, the study reports on trilayer electroactive LCE (eLCE) by intimate combination of LCE and ionic electroactive polymer device (i‐EAD). This eLCE is bi‐functional and can perform either bending or contractile deformations by the control of the low‐voltage stimulation. By applying a voltage of ±2 V at 0.1 Hz, the redox behavior and associated ionic motion provide a bending strain difference of 0.80%. Besides, by applying a voltage of ±6 V at 10 Hz, the ionic current‐induced Joule heating triggers the muscle‐like linear contraction with 20% strain for eLCE without load. With load, eLCE can lift a weight of 270 times of eLCE‐actuator weight, while keeping 20% strain and affording 5.38 kJ·m −3 work capacity. This approach of combining two smart polymer technologies (LCE and i‐EAD) in a single device is promising for the development of smart materials with multiple degrees of freedom in soft robotics, electronic devices, and sensors.