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Coating metal–organic frameworks (MOFs) on metal substrates is an important research orientation in the applications of MOFs. However, the existing binder‐based coating method needs repetitive operations and unavoidably plugs the pores of MOFs, resulting in a reduction of the adsorption capacity. Herein, a binder‐free method is proposed to construct the MOF‐on‐metal structure. The well‐intergrown...