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Abstract Chiral spin textures, as exotic phases in magnetic materials, hold immense promise for revolutionizing logic, and memory applications. Recently, chiral spin textures have been observed in centrosymmetric magnetic insulators (FMI), due to an interfacial Dzyaloshinskii–Moriya interaction (iDMI). However, the source and origin of this iDMI remain enigmatic in magnetic insulator systems. Here, the source and origin of the iDMI in Pt/Y3Fe5O12 (YIG)/substrate structures are deeply delved by examining the spin‐Hall topological Hall effect (SH‐THE), an indication of chiral spin textures formed due to an iDMI. Through carefully modifying the interfacial chemical composition of Pt/YIG/substrate with a nonmagnetic Al3+ doping, the obvious dependence of SH‐THE on the interfacial chemical composition for both the heavy metal (HM)/FMI and FMI/substrate interfaces is observed. The results reveal that both interfaces contribute to the strength of the iDMI, and the iDMI arises due to strong spin−orbit coupling and inversion symmetry breaking at both interfaces in HM/FMI/substrate. Importantly, it is shown that nonmagnetic substitution and interface engineering can significantly tune the SH‐THE and iDMI in ferrimagnetic iron garnets. The approach offers a viable route to tailor the iDMI and associated chiral spin textures in low‐damping insulating magnetic oxides, thus advancing the field of spintronics.

Abstract Multiferroic materials with flexibility are expected to make great contributions to flexible electronic applications, such as sensors, memories, and wearable devices. In this work, super‐flexible freestanding BiMnO3 membranes with simultaneous ferroelectricity and ferromagnetism are synthesized using water‐soluble Sr3Al2O6 as the sacrificial buffer layer. The super‐flexibility of BiMnO3 membranes is demonstrated by undergoing an ≈180° folding during an in situ bending test, which is consistent with the results of first‐principles calculations. The piezoelectric signal under a bending radius of ≈500 µm confirms the stable existence of electric polarization in freestanding BiMnO3 membranes. Moreover, the stable ferromagnetism of freestanding BiMnO3 membranes is demonstrated after 100 times bending cycles with a bending radius of ≈2 mm. 5.1% uniaxial tensile strain is achieved in freestanding BiMnO3 membranes, and the piezoresponse force microscopy (PFM) phase retention behaviors confirm that the ferroelectricity of membranes can survive stably up to the strain of 1.7%. These super‐flexible membranes with stable ferroelectricity and ferromagnetism pave ways to the realizations of multifunctional flexible electronics.