In this paper, we prepared a novel reactor with switchable ability to address present challenges in tandem catalyst. By introducing mussel-inspired moiety, this goal was achieved via preparing a “smart” polymer reactor which can open or closes the entry tunnel of the targeted substrate in cascade reactions. The catalyst consisted of two functional layers acting as tandem catalytic parts and one smart layer with musselinspired moieties as a controlled middle switch. The top and the bottom layer were made of molecularly imprinted polymers and catalytic components, like acidic parts and metal nanoparticles, respectively. The middle layer made of polymeric dopamine (PDPA) and acrylamide with self-healing ability will allow or inhibit the intermediate product for the reaction, thus controlling the process of the tandem catalysis. As a result, the novel catalyst exhibited self-controlled tandem catalysis, which provides new opportunities to design smart tandem catalysts, showing a promising prospect in this area.