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Fabricating mechanically responsive actuators that can efficiently convert external stimuli into mechanical work is of great significance for real‐world applications. Herein, we rationally design a class of rigid–flexible coupling crystalline crosslinked polymers (CCPs) to fabricate vapomechanically responsive actuators. Interfacial condensation reactions of flexible macromers with rigid monomers afford a series of freestanding CCP membranes. Notably, it is the first example where crosslinked polymers show high crystallinity and porosity. Moreover, the CCP membranes exhibit good mechanical properties and interesting vapor‐triggered actuation performance, which is reversible and repeatable. We find that the unusual polymer structures, high vapor sorption, and anisotropic membranes contribute to the directional deformation performance of the CCP actuators. The synthesis approach in this work provides new insights into the design and fabrication of smart materials for advanced applications. [ABSTRACT FROM AUTHOR]

Traditional ozone sensing and removal materials still suffer from high energy consumption and low efficiency. Thus, seeking new ozone‐responsive materials with high efficiency and broad working conditions is of great significance. Herein, we first developed covalent organic frameworks (COFs) for smart sensing and efficient removal of ozone. Notably, imine‐based COFs possess dramatically fast optical responses (<1 s) to ozone as low as 0.1 ppm under broad working conditions (e.g., in the presence or absence of moisture, room temperature). Moreover, we found that imine‐based COFs can also be applied as excellent ozone removers that can efficiently reduce the ozone concentration below the recommended safety limit (<0.1 ppm) for humans. The mechanism for the performance of imine‐based COFs was unveiled in‐depth by various characterization techniques and analyses. This study not only provides a new type of advanced materials for ozone sensing and removal but also broadens the application scope of COFs. [ABSTRACT FROM AUTHOR]