In recent years, significant progresses have been recorded in the development of soft actuators regarding the material and structural designs. [11,[13][14][15][16][17] Improved actuation speed was obtained by decreasing the response time of volume change; [9][10][11][18][19][20] and enhanced actuation force was realized by increasing the rigidity of the actuator material; [19,[21][22][23][24][25][26] and increased bending curvature was achieved by increasing the asymmetric volume change. [27,28] For example, fast response can be realized employing the following strategies, for example, by increasing absorption/desorption of vapor molecules by the actuator film, [18][19][20] or by increasing the shrinking of the film by photothermal-induced water-desorption, [9,10] or by increasing polymer volume expansion via the photothermal effect of carbon nanomaterials. [11] The bimorph actuators fabricated from soft materials (e.g., elastomers and hydrogels) commonly exhibit a larger bending curvature, [29][30][31] but lower actuation force and response rate compared with those fabricated from rigid materials. Contrarily, the rigidmaterial-based actuators can generate relatively faster actuation speed and larger force, [16,21,25] but smaller bending curvature compared to those fabricated from soft materials. Therefore, it is challenging to simultaneously achieve high actuation force and large bending curvature within a short response time.Until now, there are only a few successful designs of thinfilm jumping actuators by different delicate approaches. [9][10][11][12] Aida group reported a π-stacked carbon nitride polymer (CNP) thin film actuator exhibiting a tough, ultra-lightweight and highly anisotropic layered structure, which responded to the adsorption and desorption of a minute amount of water and is extremely rapid (50 ms by one curl). The film can jump 10-mmhigh on light irradiation by losing the adsorbed water. [10] Wang group reported graphene oxide (GO)/CNT bilayer actuator, where the GO layer allowed fast diffusion of water molecules and the aligned CNT layer imposed constrain. The actuator showed fast response (0.08 s) with large bending curvature, which demonstrated jumping actuation under photothermal induced water desorption from the GO layer. [9] Chen and coworkers prepared a jumping actuator by mimicking flicking finger motion, employing the rolled CNT/polydimethylsiloxane (PDMS) bilayer composite. The unique combination of loosely CNT network, good photo-thermal effect of CNT, and the large difference between thermal expansion coefficient between the two layers resulted in light-induced jumping up to five times higher than its own height. [11] Cai group reported a jumping actuator by mimicking the fruit fly larva, employing CNT/ liquid crystal elastomer (LCE) bilayer composite. Under light It is highly desirable to develop compact-and robust-film jumping robots that can withstand severe conditions. Besides, the demands for strong actuation force, large bending curvature in a short response time, and good e...