A humidity-responsive bilayer actuator has been developed that consists of an oriented polyamide-6 substrate and a liquid-crystalline polymer coating. The oriented substrate acts as an alignment layer for the liquid crystal. The liquid-crystalline polymer consists of a supramolecular network having hydrogen-bonded entities that, after activation with an alkaline solution, exhibit deformation in response to a change in humidity. The bending behavior of the bilayer actuator was analyzed, showing a large response to a change in the humidity.