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Abstract Carbon nanocoils (CNCs), with quasi‐1D morphology and unique helical structure, are found to have great potential as nanocantilevers for multifunctional micro/nano electro‐mechanical devices and systems. Instead of conventional mechanical actuation, photo‐actuation is a high‐efficient and low‐power‐consuming approach with the advantages of remote control and possible utilization of solar energy. This work investigates the photo‐mechanics of CNC‐based cantilever. An “enhancement of photo‐mechanical response” effect is found, which comes from the photothermal coupling between CNC and surrounding environment. Moreover, for curving CNCs, the photo‐induced vibration of CNC cantilever is strongly modulated through regulating the laser‐irradiation position. The amplitude‐to‐length ratio increases nearly five‐fold, from 0.05 to 0.24. CNC‐based nanocantilevers have promising applications in photo‐controlled thermal generators and photo‐driven actuators.