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Here, the actuation response of an architectured electrothermal actuator comprising a single layer of carbon nanotube (CNT) film and a relatively thicker film of silk, cellulose, or polydimethylsiloxane is studied. An electric current is passed through the CNT film, which generates heat responsible for electrothermal actuation, in all samples, affixed as per doubly clamped beam configuration. All samples, including pure CNT film, show remarkable actuation such that actuation monotonically increases with the applied voltage. Cyclic pulsed electrical loading shows a lag in the electric current stimulus and the actuation. Remarkably, an ultrahigh actuation of ∼2.8%, which was 72 times more than that shown by pure CNT film, is measured in the CNT-cellulose film, that is, the architectured actuator with the natural polymer having the functional property of hygroexpansion and the structural hierarchy of the CNT film, however, at a significantly larger length scale. Overall, the synergetic contribution of the individual layers in these bilayered actuators enabled achieving ultrahigh electrothermal actuation compared to the homogeneous, synthetic polymer-based devices. A detailed discussion, which also includes examination of the role of the hierarchical substructure and the functional properties of the substrate and numerical analysis using the finite element method, is presented to highlight the actuation mechanism in the fabricated actuators.

Deterministic Role of Carbon Nanotube-Substrate Coupling for Ultrahigh Actuation in Bilayer Electrothermal Actuators