A new type of soft actuators based on a vertical stack of nanoporous 2,2,6,6‐tetramethylpiperidine‐1‐oxyl‐oxidized cellulose nanofibers (TOCNs) and atomically thin 2D platinum ditelluride (PtTe₂) layers is reported. The actuation of TOCNs is driven by the interfacing 2D PtTe₂ layers whose electrothermal proficiency precisely controls their hydration/dehydration states sensitive to mechanical deformation. These vertically stacked TOCN/2D PtTe₂ actuators present excellent actuation characteristics such as high linearity of bending curvature versus applied voltage and well‐preserved reversibility during cyclic operations. Most notably, they exhibit an extremely large weight‐lifting ratio, i.e., ≈1000 times the mass of the TOCN layers, confirming superior mechanical robustness. Furthermore, complicated actuations such as twisting in a 3D manner are demonstrated by judiciously controlling the surface wettability of TOCN layers. This study unveils opportunities for CNFs and 2D materials for actuator applications, as well as suggests new design strategies broadly applicable to soft robotics and biomimetic devices.