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The fabrication of MOF polymer composite materials enables the practical applications of MOF‐based technology, in particular for protective suits and masks. However, traditional production methods typically require organic solvent for processing which leads to environmental pollution, low‐loading efficiency, poor accessibility, and loss of functionality due to poor solvent resistance properties. For the first time, we have developed a microbial synthesis strategy to prepare a MOF/bacterial cellulose nanofiber composite sponge. The prepared sponge exhibited a hierarchically porous structure, high MOF loading (up to ≈90 %), good solvent resistance, and high catalytic activity for the liquid‐ and solid‐state hydrolysis of nerve agent simulants. Moreover, the MOF/ bacterial cellulose composite sponge reported here showed a nearly 8‐fold enhancement in the protection against an ultra‐toxic nerve agent (GD) in permeability studies as compared to a commercialized adsorptive carbon cloth. The results shown here present an essential step toward the practical application of MOF‐based protective gear against nerve agents.

Wearable personal protective equipment that is decorated with photoactive self‐cleaning materials capable of actively neutralizing biological pathogens is in high demand. Here, we developed a series of solution‐processable, crystalline porous materials capable of addressing this challenge. Textiles coated with these materials exhibit a broad range of functionalities, including spontaneous reactive oxygen species (ROS) generation upon absorption of daylight, and long‐term ROS storage in dark conditions. The ROS generation and storage abilities of these materials can be further improved through chemical engineering of the precursors without altering the three‐dimensional assembled superstructures. In comparison with traditional TiO₂or C₃N₄self‐cleaning materials, the fluorinated molecular coating material HOF‐101‐F shows a 10‐ to 60‐fold enhancement of ROS generation and 10‐ to 20‐fold greater ROS storage ability. Our results pave the way for further developing self‐cleaning textile coatings for the rapid deactivation of highly infectious pathogenic bacteria under both daylight and light‐free conditions.