An　oscillatory　pH　system　is　implemented　to　drive　oscillatory　pH-switchable　DNA　machines　and　to　control　pH-stimulated　electron　transfer　at　electrode　surfaces.　The　oscillatory　pH　system　drives　the　autonomous　opening　and　closure　of　DNA　tweezers　and　activates　a　DNA　pendulum　by　the　pH-stimulated　formation　and　dissociation　of　i-motif　structures.　Also,　a　sequence-programmed　nucleic　acid　monolayer-functionalized　electrode　undergoes　autonomous　oscillatory　pH　transitions　between　random　coil　and　i-motif　configurations,　leading　to　the　control　of　electron　transfer　at　electrode　surfaces.　©　2013　American　Chemical　Society.