Perpendicular magnetic anisotropic materials are of great interest for their huge potential to realize high‐density non‐volatile memory and logic chips. Designing such materials with lower cost and better magnetoelectric coupling still remains major challenges. In this work, aurivillius oxide ceramics with highly [00l]‐oriented grains were prepared by a facile pressureless sintering method, and the perovskite layer number was modified by varying the cobalt content. Afterwards, the unique perpendicular magnetic anisotropy and the intriguing anisotropic ferroelectric properties have been observed. The magnetic properties of the aurivillius oxides with different layer numbers have been carefully investigated by field cooling, zero field cooling, and the magnetization with a varying field. The magnetic anisotropy in the oriented ceramics is demonstrated to be caused by the magnetocrystalline anisotropy with the easy magnetization direction along the c‐axis, which possibly arises from the unquenched 3d orbitals combined with the special layered crystal structures. The magnetocrystalline anisotropy becomes weaker in the ceramics with lower‐numbered perovskite layers, while the orientation degree of the ceramics and the ferroelectric anisotropy show quite opposite trends. Furthermore, the weak magnetoelectric coupling is also observed in the ceramics. This special anisotropic multiferroic properties may open up a new window for the aurivillius materials.
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