Ferritin-based nanofibrous hydrogels that clearly demonstrate synergy between the ferritin protein and the synthetic polymer matrix was fabricated. The hybrid hydrogels showed enhanced mechanical properties and repeated expansion and contraction without showing severe creep during pH switching. About 0.4 g of PVA was dissolved in 4.9mL DI water, and then the mixture was stirred for 1 h at 90°C, before being allowed to cool to room temperature. A voltage of 10 kV was applied between the syringe needle and the grounded aluminum electrodes using a high-voltage power supply. The syringe needle acted as an anode and the aluminum electrode acted as a cathode. The distance between the syringe needle and the aluminum electrode was 12 cm. It was observed that the ferritin nanoparticles act as nanosprings, which connect the polymer matrix and ferritin core via hydrogen bonds formed by functional groups of the ferritin and PVA.