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Abstract The engineering of metal–organic frameworks (MOFs) into membranes and films is being investigated, to transform laboratory‐synthesized MOFs into industrially viable products for a range of attractive applications. However, rational design and construction of highly permeable MOF thin films, without trade‐offs in terms of structural mechanical stability, remains a significant challenge. Herein, a simple, general strategy is reported to prepare thin MOF nanosheet (NS)‐assembled frame film via heteroepitaxial growth from metal hydroxide film. As the thin MOF NS‐assembled film significantly enhances the permeability of mass though the film, the resultant gold nanoparticle (Au NP)@MOF film exhibits much higher catalytic efficiency than the Au NP@MOF bulk film. Meanwhile, the unique framework of the MOF NS‐assembled film resists torsion and collapse, so the composite catalyst exhibits long‐term stability.

The engineering of metal–organic frameworks (MOFs) into membranes and films is being investigated, to transform laboratory‐synthesized MOFs into industrially viable products for a range of attractive applications. However, rational design and construction of highly permeable MOF thin films, without trade‐offs in terms of structural mechanical stability, remains a significant challenge. Herein, a simple, general strategy is reported to prepare thin MOF nanosheet (NS)‐assembled frame film via heteroepitaxial growth from metal hydroxide film. As the thin MOF NS‐assembled film significantly enhances the permeability of mass though the film, the resultant gold nanoparticle (Au NP)@MOF film exhibits much higher catalytic efficiency than the Au NP@MOF bulk film. Meanwhile, the unique framework of the MOF NS‐assembled film resists torsion and collapse, so the composite catalyst exhibits long‐term stability. [ABSTRACT FROM AUTHOR]