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Insulating uniaxial room‐temperature ferromagnets are a prerequisite for commonplace spin wave‐based devices, the obstacle in contemporary ferromagnets being the coupling of ferromagnetism with large conductivity. It is shown that the uniaxial  A  1 + 2   x  Ti 4+  1 −    x  O 3  (ATO),  A  = Ni 2+ ,Co 2+ , and 0.6 <  x  ≤ 1, thin films are electrically insulating ferromagnets already at room temperature. The octahedra network of the ATO and the corundum and ilmenite structures are the same yet different octahedra‐filling proved to be a route to switch from the antiferromagnetic to ferromagnetic regime. Octahedra can continuously be filled up to  x  = 1, or vacated (−0.24 <  x  < 0) in the ATO structure. TiO‐layers, which separate the ferromagnetic (Ni,Co)O‐layers and intermediate the antiferromagnetic coupling between the ferromagnetic layers in the NiTiO 3  and CoTiO 3  ilmenites, can continuously be replaced by (Ni,Co)O‐layers to convert the ATO‐films to ferromagnetic insulator with abundant direct cation interactions.

Room‐Temperature Insulating Ferromagnetic (Ni,Co) 1+2 x Ti 1− x O 3 Thin Films