“…[ 4–7 ] These alterations result in an interfacial region typically of order 2–10 unit cells in which the octahedral rotations are suppressed, enhanced, or even take on different patterns than found in either of the adjoined materials. [ 8–13 ] As the orbital hybridization between the B‐site‐derived d states and O 2p states is linked to the BOB bond angles and lengths, the electronic, magnetic, and optical functionality at perovskite interfaces is highly sensitive to the structural distortions. In magnetic oxide heterostructures, interfacial octahedral coupling has been shown to directly influence local magnetization, [ 14–19 ] ordering temperatures, [ 20,21 ] and magnetocrystalline anisotropy.…”