Emerging 2D magnetic heterojunctions attract substantial interest due to their potential applications in spintronics. Achieving magnetic phase engineering with structural integrity in 2D heterojunctions is of paramount importance for their magnetism manipulation. Herein, starting with chromium ditelluride (CrTe2) as the backbone framework, various lateral and vertical magnetic heterojunctions are obtained via self‐intercalated 2D chromium telluride (CrxTey). A Cr2Te3‐Cr5Te8 lateral heterojunction prototype is demonstrated for the manipulation of magnetic moments under different magnitudes of magnetic excitation, showing a sharply stepped hysteresis loop with a dual spin‐flip transition at high Curie temperatures up to 150 and 210 K by magneto‐optical Kerr measurement. High‐resolution scanning transmission electron microscopy and first‐principles calculations reveal a preferred random location of Cr intercalants at the phase boundary, allowing lowering energy associated with crystal field splitting. The overall structural rigidity of chromium‐telluride heterostructure with magnetic phase decoupled behaviors is promising for 2D spintronic devices.

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The flexomagnetic effect involves the coupling of inhomogeneous mechanical and magnetic excitations to generate exotic spin orders. The intrinsic edge stress associated with lifting of periodic degeneracy at surfaces or edges in nanostructures facilitates the flexocoupling effects. Here, we combine first-principles calculation and Maximum Information Coefficient (MIC) statistics to quantitatively reveal the impact of bending on the geometries, spin ordering state, and exchange interactions in chromium triiodide (CrI3) nanoribbons. Our results reveal a divergent magnetic ground state at small curvature but a plumb line shape noncollinear state at large curvatures. More importantly, our work establishes a gradient dependence of the exchange coupling on the locally asymmetric bending angles of the Cr-I-Cr hinge, governed by the coupling of the t2g and eg states of Cr. The superexchange gradient accompanied with the bending-induced inhomogeneous deformation sheds light on the evolution of magnetic ordering associated with asymmetric coordinating systems for sensors and spintronics.