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The indoor air quality is of prime importance for human daily life and health, for which the adsorbents like zeolites and silica‐gels are widely used for air dehumidification and harmful gases capture. Herein, we develop a pore‐nanospace post‐engineering strategy to optimize the hydrophilicity, water‐uptake capacity and air‐purifying ability of metal‐organic frameworks (MOFs) with long‐term stability, offering an ideal candidate with autonomous multi‐functionality of moisture control and pollutants sequestration. Through variant tuning of organic‐linkers carrying hydrophobic and hydrophilic groups in the pore‐nanospaces of prototypical UiO‐67, a moderately hydrophilic MOF (UiO‐67‐4Me‐NH2‐38 %) with high thermal, hydrolytic and acid‐base stability is screened out, featuring S‐shaped water sorption isotherms exactly located in the recommended comfortable and healthy ranges of relative humidity for indoor ventilation (45 %–65 % RH) and adverse health effects minimization (40–60 % RH). Its exceptional attributes of water‐uptake working capacity/efficiency, contaminants removal, recyclability and regeneration promise a great potential in confined indoor environment application. [ABSTRACT FROM AUTHOR]

The design and creation of soft porous crystals combining regularity and flexibility may promote potential applications for gas storage and separation due to their deformable framework's responsiveness to external stimuli. The flexibility of metal–organic frameworks (MOFs) relies on alterable degrees of freedom that are mainly provided by organic linkers or the junctions linking organic and inorganic building units. Herein, we report a new dynamic MOF whose flexibility originates from an unprecedented tailorable Mn8O38‐cluster and shows simultaneous coordination geometry changes and ligand migration that are reversibly driven by guest exchange. This provides an extra degree of freedom to the framework's deformation, resulting in three‐dimensional variations in the framework that subtly respond to varied aromatic molecules. The gas adsorption behavior of this flexible MOF was evaluated, and the selective separation of light hydrocarbons and Freon gases is achieved. [ABSTRACT FROM AUTHOR]