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A strong anisotropic magnetoresistance (AMR) effect induced by spin–orbit coupling is the basis for constructing a highly sensitive and reliable magnetic sensor. Presently, effective AMR enhancement in traditional films focuses on the modulation of the lattice or charge degree of freedom, leading to a general AMR ratio below 4%. Here, we demonstrate a different strategy to strengthen the AMR effect by tuning the orbital degree of freedom. By inserting an oxygen-affinitive Hf layer into a Ta/MgO/NiFe/MgO/Ta multilayer film, Fe–O orbital hybridization at the MgO/NiFe interface was modulated to trigger an effective orbital reconfiguration of Fe. In turn, the number of holes in the in-plane symmetric d orbits of Fe increased substantially, facilitating the s–d electron scattering to enhance the AMR ratio to 4.8%. By further micromachining the film into a Wheatstone bridge, we constructed a sensing element that displayed an ultrahigh sensitivity of 2.7 mV/V/Oe and a low noise detectability of 0.8 nT/√Hz. These findings help to advance the development of orbit-governed AMR sensors and provide an alternative method for tuning other orbit-related physical effects.

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