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This study is aimed at the present challenge in tandem catalysts, addressing how to endow the catalysts with self‐controlled tandem catalytic‐ability. By borrowing the predation strategy from sundew, the objective was originally met by reporting a smart tandem catalyst which can self‐control the tandem catalytic behavior by catching, decomposing and assimilating the engaging molecules (such as 4‐nitrophenyl acetate). This catalyst was made of a unique leaf containing two functional layers where each may be responsible for one coupled process. The first layer in this catalyst was fabricated with a zipper‐like reactive polymer capable of opening and closing, which allowed the catalyst to catch and decompose 4‐nitrophenyl acetate. The second layer in this catalyst allowed, however, further access to assimilate the decomposed substrate (i. e., 4‐nitrophenol), made of an antibody‐like polymer and encapsulated metal nanoparticles. In this way, the use of this catalyst led to the occurrence of the self‐controlled tandem catalytic‐ability. This novel design suggests a new protocol for developing smart tandem catalysts, which opens new opportunities for controlled tandem catalytic processes. Copying Nature: Inspired by the predation strategy in sundews, this study presents the first case of smart tandem catalysts which can self‐control the tandem catalytic behavior by catching, decomposing and assimilating the engaging molecules (such as 4‐nitrophenyl acetate). This catalyst was fabricated with a unique leaf made of two functional layers where each may be responsible for one coupled process. This novel design opens new opportunities for controlled tandem catalytic processes. [ABSTRACT FROM AUTHOR]