Abstract We report exceptionally large tunnel magnetoresistance (TMR) for biomolecular tunnel junctions based on ferritins immobilized between Ni and EGaIn electrodes. Ferritin stores iron in the form of ferrihydrite nanoparticles (NPs) and fulfills the following roles: (a) it dictates the tunnel barrier, (b) it magnetically decouples the NPs from the ferromagnetic (FM) electrode, (c) it stabilizes the NPs, and (d) it acts as a spin filter reducing the complexity of the tunnel junctions since only one FM electrode is required. The mechanism of charge transport is long-range tunneling which results in TMR of 60 ± 10% at 200 K and 25 ± 5% at room temperature. We propose a magnon-assisted transmission to explain the substantially larger TMR switching fields (up to 1 Tesla) than the characteristic coercive fields (a few Gauss) of ferritin ferrihydrite particles at T < 20 K. These results highlight the genuine potential of biomolecular tunnel junctions in designing functional nanoscale spintronic devices.