In this study, we succeeded in manufacturing a novel nanofiber hydrogel actuator that caused a bending and stretching motion synchronized with external pH oscillation, based on a bromate/sulfite/ferrocyanide reaction. The novel nanofiber gel actuator was composed of electrospun nanofibers synthesized by copolymerizing acrylic acid and hydrophobic butyl methacrylate as a solubility control site. By changing the electrospinning flow rate, the nanofiber gel actuator introduced an anisotropic internal structure into the gel. Therefore, the unsymmetrical motion of the nanofiber actuator was generated.