Ferritin-based nanofibrous hydrogels that demonstrate synergy between the ferritin protein and the synthetic polymer matrix are fabricated. The hybrid hydrogels showed enhanced mechanical properties and repeated expansion and contraction without showing severe creep during pH switching. The ferritin nanoparticles incorporated into the hydrogel nanofibers improved the actuation stability of a hydrogel actuator by acting as elastic nanosprings in a nanoscale polymer.