AbstractPreparation and low voltage induced bending (converse flexoelectricity) of crosslinked poly(ethylene glycol) diacrylate (PEGDA), modified with thiosiloxane (TS) and ionic liquid (1‐hexyl‐3‐methylimidazolium hexafluorophosphate) (IL) are reported. In between 2µm PEDOT:PSS electrodes at 1 V, it provides durable (95% retention under 5000 cycles) and relatively fast (2 s switching time) actuation with the second largest strain observed so far in ionic electro‐active polymers (iEAPs). In between 40 nm gold electrodes under 8 V DC voltage, the film can be completely curled up (270° bending angle) with 6% strain that, to the best of the knowledge, is unpreceded among iEAPs. These results render great potential for the TS/PEGDA/IL based electro‐active actuators for soft robotic applications.