magnetic field. From the discovery of electromagnetic induction to the quantum Hall effect, humans have strived for seeking applicability of novel mechanisms in the magneto-sensors. [2] Currently, the magneto-sensors are generally based on the quantum effects, which relies on a highly sensitive interface of semiconductor materials commonly fabricated by epitaxial growth. [3] With development of flexible electronics and bioelectronics, these semiconductor based technics seem increasingly unsuitable for the biomedical applications.Interestingly, some species possess an amazing capability of magneto-perception such as migratory birds, [4] butterflies, [5] and honeybees. [6] These animals perceive the geomagnetic field relying on special proteins. Cryptochrome (Cry) has been considered for a long time to mediate the magneto-perception via quantum spin dynamics of light-induced radical-pair, which are excited by sunlight and can be modulated by the geomagnetic field. [7][8][9] This principle was employed to sense the magnetic field because the life-time and the spectral characteristic of radical pair in singlet and triplet states can reflect the information about magnetic field. [10] Cry played an important role in the During billions of years of evolution, some species develop fantastic magnetoperception, offering a biomimetic route to develop the next generation of magneto-sensors. Recently, a novel principle was proposed to explain the navigation of pigeons in the presence of geomagnetic fields and sunlight. The key link is thought to lie in the magneto-optically involved conformational variation of magnetoreceptor protein (MagR)/cryptochrome (Cry4) complex. The MagR/Cry4 complex is fabricated and purified in vitro, creating a magnetosensing device by immobilization of this protein on a graphene-modified electrochemical electrode. By using electrochemical impedance spectroscopy, magneto-sensing with a current detectability of 10 mT is realized with MagR/ Cry4 complex. It is proved that this process requires the involvement of both magnetic fields and light, partly confirming in vitro the magneto-perceptive mechanism of MagR/Cry4 complex. It is also shows that this device can be used to reflect the anisotropic responses of nanomaterials to the external magnetic field. It is believed this protein-based magneto-sensing will greatly boost development of bioelectronics and deepen understanding of the phenomena of magneto-perception for organisms.