LAUSR

Breaking time‐reversal symmetry by introducing magnetic order, thereby opening a gap in the topological surface state bands, is essential for realizing useful topological properties such as the quantum anomalous Hall and axion insulator states. In this work, a novel topological antiferromagnetic (AFM) phase is created at the interface of a sputtered, c‐axis‐oriented, topological insulator/ferromagnet heterostructure—Bi2Te3/Ni80Fe20 because of diffusion of Ni in Bi2Te3 (Ni‐Bi2Te3). The AFM property of the Ni‐Bi2Te3 interfacial layer is established by observation of spontaneous exchange bias in the magnetic hysteresis loop and compensated moments in the depth profile of the magnetization using polarized neutron reflectometry. Analysis of the structural and chemical properties of the Ni‐Bi2Te3 layer is carried out using selected‐area electron diffraction, electron energy loss spectroscopy, and X‐ray photoelectron spectroscopy. These studies, in parallel with first‐principles calculations, indicate a solid‐state chemical reaction that leads to the formation of Ni−Te bonds and the presence of topological antiferromagnetic (AFM) compound NiBi2Te4 in the Ni‐Bi2Te3 interface layer. The Neél temperature of the Ni‐Bi2Te3 layer is ≈63 K, which is higher than that of typical magnetic topological insulators (MTIs). The presented results provide a pathway toward industrial complementary metal−oxide−semiconductor (CMOS)‐process‐compatible sputtered‐MTI heterostructures, leading to novel materials for topological quantum devices.