Amorphous carbon nitride (a-CNx) thin films deposited by reactive sputtering have great potential for driving source applications of light-driven active devices. We demonstrate, for the first time, the photoinduced deformation of a-CNx deposited on flexible substrates, namely, poly(ethylene naphthalate) (PEN) films and transparent cellulose nanopaper. a-CNx films without delamination were obtained on both substrates. By decreasing the thickness of PEN films, the photoinduced deformation became extremely large. A light-driven pump was fabricated using a-CNx-coated PEN films, and then the pumping motion was observed up to 10 Hz. When a He-Ne laser traced the surface of a-CNx films deposited on the nanopaper, the sample moved to the opposite side of the laser spot. The motion involved repeated expansions and contractions similar to the motion of caterpillars occurring owing to the temporary photoinduced deformation of a-CNx films.