Although responsive actuators have been intensively investigated, it remains challenging to enable rapid and self-oscillating actuation under ambient circumstances without human intervention analogous to living organisms. By hybridizing a unique type of two-dimensional nanomaterials (i.e., MXene) with a particular hydrophilic polymer, a smart and flexible conductive composite was produced with rapid actuation and spontaneous oscillation near a moist surface. Due to the presence of layered microstructures and the moisture-sensitivity improved by surface roughness and intercalated polymeric layers, the composites could reversibly bend up to 180° in 2 s or 210° in 10 s on demand when the circumstantial humidity was varied, being superior or comparable to many actuators in the literature. More importantly, the composite was capable not only of flipping upside down repeatedly on the moist surface but also of self-oscillating ceaselessly under ambient gradient humidity without human intervention, e.g., an oscillation between 30 and 100° with an oscillation frequency of 0.08 Hz. This self-oscillation resulted from the occurrence of rapid asymmetrical hydration and dehydration of the composite between the regions of high and low humidity, which could further be modulated both by different hydrophilic polymers and by photoradiation owing to the photothermal effect of MXene nanosheets. Because of the ubiquitous presence of humidity gradient near the moist surface, this type of smart composite may not only offer a strategy for designing artificial materials that are capable of spontaneous actuation under ambient circumstance without human intervention but also promise potential applications in artificial muscles, autonomous robotics, and energy harvesting from environments.