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An actuating system composed of nafion ionomeric polymer coated with single-walled carbon nanotubes electrodes was studied as an electromechanical actuator. The actuator gives a sizable mechanical response to low voltages (turn-on voltage of ∼2.5 V) under open-air conditions, i.e., in the absence of a surrounding supporting electrolyte. The actuator is active under both dc and ac bias and has a strong resonance at low frequencies which is dependent upon the size of the actuator. The actuator was studied using Fourier transform infrared and vis-NIR spectroscopies, cyclic voltammetry, and by the current-time response under an applied step voltage. An analytical model is proposed to understand the electrical behavior, which is consistent with the spectroscopic results.