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Inspired by efficient biomolecular reactions in the cell, versatile DNA nanostructures have been explored for manipulating the spatial position and regulating reactions at the molecular level. Spatially controlled arrangement of molecules on the artificial scaffolds generally leads to enhanced reaction activities. Especially, the rich toolset of dynamic DNA nanostructures provides a potential route towards more sophisticated and vigorous regulation of molecular reactions. Herein, a reconfigurable DNA origami domino array (DODA) as a dynamic scaffold was adopted in this work for temporal‐controlled and switchable molecular cascade reactions. Dynamic regulation of the assembly of G‐quadruplex, hybridization of parallel‐stranded duplex and assembly of binary DNAzyme were demonstrated. Molecular cascade reactions on the triggered reconfiguration of DODAs were realized, resulting in more complex, dynamic, and switchable control over the reactions. [ABSTRACT FROM AUTHOR]