Bilayer actuators, traditionally consisting of two laminated materials, are the most common types of soft or hybrid actuators. Herein, a nanomaterial-based organic–inorganic humidity-sensitive bilayer actuator composed of TEMPO-oxidized cellulose nanofibrils (TCNF-Na+) and reduced graphene oxide (rGO) sheets is presented. The hybrid actuator displays a large humidity-driven locomotion with an atypical fast un-bending. Cationic exchange of the anionically charged TCNF-Na+ and control of the layer thickness is used to tune and dictate the locomotion and actuator's response to humidity variations. Assembly of a self-oscillating electrical circuit, that includes a conductive rGO layer, displays autonmous on-and-off lighting in response to actuation-driven alternating electrical heating.