Photoreactive olefinic species are incorporated into am etal-organic framework (MOF), [Zn(bdc)(3-F-spy)] (1). Single crystals of 1 are shown to undergo three types of photomechanical macroscopic deformation upon illumination by UV light. To demonstrate the practical potential of this system, the inclusion of 1 in aP VA (polyvinyl alcohol) composite membrane,b ye xploiting hydrogen-bonding interactions,i sp resented. Using this composite membrane,t he amplification of mechanical stress to achieve macroscopic actuation behavior is demonstrated. These results pave the way for the generation of MOF-based soft photoactuators that produce clearly defined mechanical responses upon irradiation with light. Such systems are anticipated to have considerable potential in photomechanical energy harvesting and conversion systems.Actuation materials that effectively convert external controllable stimuli into mechanical energy have recently attracted attention in the fields of soft robotics, [1] biomedicine, [2] biomimetic systems, [3] and molecular machines, [4] with synthetic materials having the potential to undergo intended deformations involving twisting,b ending,s wimming,a nd elongation/contraction. [5] Va rious types of smart actuation driven by external physical or chemical stimuli (for example, heat, [6] electricity, [7] magnetism, [8] humidity, [9] or light [10] )have been extensively investigated and developed. Thedesign and fabrication of as mart actuation that can achieve multiple desired deformations and perform target functions are essential prerequisites. [4,11] Accordingly,t he manipulation and deformation of actuation associated with rapid and precise response is of great relevance to both fundamental research and practical applications toward the prompt and Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.