crucial for application in functional spintronic devices and high-density magnetic recording technology. [3][4][5][6][7] To explore or synthesize magnetic materials with high coercivity, materials with large MAs are required for obtaining high-performance permanent magnets. Because MA is indirectly proportional to the symmetry of the crystal, materials with lower crystal symmetry are promising for application as high-MA compounds. Generally, the physical origin of large MAs is spin-orbit interaction (SOI), calculated as the inner product of orbital (L ) and spin angular momenta (S) with an interaction constant λ. For a given spin moment, the magnitude of SOI is determined by λ and the expected value of the orbital angular momentum. Magnetic materials composed of noble metals often exhibit large MAs, attributed to the large λ values of noble metals. In contrast, the large MAs of permanent magnets composed of rare-earth elements are attributed to their large values of λ and orbital angular momenta. [3,[8][9][10][11][12][13] In transition metal alloys or compounds that do not contain heavy or rare-earth elements, L is often quenched in a crystal field. Consequently, magnetic materials with large MAs are rare. In contrast, a certain amount of orbital angular momentum is sometimes retained in oxides, owing to the localized character of the wave functions of transition metal ions in the crystal field. The magnitude of the orbital angular momentum is influenced by the electronic configurations of the magnetic ions; therefore, the MAs of magnetic oxides can be induced/enhanced by introducing asymmetry, such as lattice deformations. This phenomenon can be considered to be magneto-elastic in nature because the change in magnetic state is induced by lattice deformation. Furthermore, a large uniaxial MA can be realized by uniaxial lattice deformation. The epitaxial distortion arising from the lattice mismatch between oxide thin films and their substrates can be employed to effectively induce lattice distortion.Co x Fe 3−x O 4 (CFO) has a cubic lattice, as shown in Figure 1a, and exhibits a large cubic MA with a Néel temperature of 769 K for x = 1.0 and has been reportedly used as permanent magnets. [14] Extensive magneto-elastic effects have been reported, along with the existence of a large orbital moment in Co 2+ . [15][16][17][18][19][20][21][22][23][24][25][26] The large cubic MA of bulk CFO has been elucidated theoretically using a single-ion model; the cubic and local trigonal lattice symmetries split the down-spin t 2g state into a singly Perpendicular magnetic anisotropy (PMA) energy up to K u = 6.1 ± 0.8 MJm −3 is demonstrated in this study by inducing large lattice distortion exceeding 3% at room temperature in epitaxially distorted cobalt ferrite Co 0.73 Fe 2.18 O 4 (001) thin films. Although the thin film materials include no rare-earth elements or noble metals, the observed K u is larger than that of the neodymium-iron-boron compounds for high-performance permanent magnets. The large PMA is attributed to the sig...