Smart shape-memory DNA hydrogels, which can respond to various types of external stimuli and undergo macroscopic shape deformations, have shown great potential in various applications. By constructing free-standing films, the deformation and response properties of these hydrogels can be further enhanced, and visualized deformation can be achieved. However, DNA hydrogels that can exhibit rapid and high-degree shape deformations, such as the inverse shape deformations, are still lacking. Herein, free-standing oligoadenine strand-functionalized polyacrylamide hydrogel films were developed that can exhibit reversible and high degree of inverse shape deformation upon cyclic pH changes. The oligoadenine strands exhibit a pH-stimulated reversible conformational transition between a flexible single-stranded state and parallel duplex A-motif structures, resulting in their role change in the film from negatively charged side chains to "head-to-head" crosslinking structures, driving a high degree of inverse shape deformation with a relative bending angle change of 223.7 % of the film, which is more than 5 times that of a film driven by pH-responsive i-motif structures, facilitating the development of bilayer hydrogel film actuators with potential in flexible sensors and robots.