Flexible magnetoelectric device is one of the indispensable elements. However, the complicated fabrication process and low sensitivity hinders the practical applications. Here, flexible NiFe anisotropic magnetoelastic composites were prepared by cluster–supersonic expansion method assistant with polyvinylidene fluoride (PVDF) substrates. The NiFe/PVDF composites possess sensitive angle–resolution magnetoelectric coupling coefficient at room temperature, and the value can reach 0.66 μV/deg. The strong anisotropic magnetoelasticity phenomenon is reminiscent of the short–range ordered cluster structure. The anisotropic magnetoelastic coefficient can be deduced by temperature– and magnetic field strength–dependent anisotropic magnetoresistance. The magnetic torque results also prove the strong anisotropic magnetoelastic trait. The coupling between piezoelectricity and anisotropic magnetostrictive effect endows great possibilities toward flexible electronic compass. These results shed light on future in non–invasive tracking of vital biological health via wearable electronic devices.

The origin of the planar Hall effect (PHE) decides an effective regulation of magnetic domain states on its performance. However, it has to suffer from the mutual interference between different kinds of domain states due to the narrow switching size range between multi-domain and single-domain states. Here, we fabricated nanostructured Ni0.8Fe0.2 alloy films assembled with the extremely narrow size distribution of clusters using the low-energy cluster beam deposition technique. It realizes an evolution from multi-domain and bi-domain to single-domain states by using its precise size-controllable characteristics. The PHE of films with the multi-domain state presents obvious hysteresis behavior, but it disappears for the single-domain state. The switching of the domain state also significantly affects the field- and angle-dependent magnitudes of the PHE. Such regulation behaviors are mainly originated from the effect of the pinning and depinning behaviors of domain walls on electron scattering. This work shows the regulation of the PHE by domain state switching in a powerful way, which is beneficial to promote its mechanism and application.