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Establishing a reliable control of perpendicular magnetic anisotropy (PMA) is challenging but essential for the full utilization of rare‐earth iron garnets in spintronic devices. In this study, a feasible approach to enhance the PMA of ferrimagnetic thulium iron garnet (TmIG) films is presented. This approach involves precise adjustments in cation stoichiometry and epitaxial strain state. By fine‐tuning the pre‐ablation process and oxygen partial pressure during pulsed laser deposition, a series of high‐quality TmIG films can grow with variable cation stoichiometry, i.e., the Tm/Fe molar ratio. The finding reveals that cation stoichiometry plays a crucial role in determining the magnetic properties of the TmIG films. Particularly, the stoichiometric TmIG film has the strongest PMA due to the maximized magnetostriction coefficient. Combining this stoichiometry optimization and strain engineering, an unprecedented PMA strength of ≈30 kJ m−3 for TmIG is achieved. This achievement demonstrates a simple and effective method for harnessing the magnetic properties of rare‐earth iron garnet films, paving the way for their advanced applications in next‐generation spintronic devices. [ABSTRACT FROM AUTHOR]

Understanding the magnetotransport properties of SrRuO3 thin films and heterostructures is essential for both fundamental research and practical applications. While the anomalous Hall effect has been studied extensively, the longitudinal magnetotransport (i.e. magnetoresistance) is not well understood and requires further investigation. Herein, SrRuO3/SrTiO3(001) epitaxial film is used as a model system to systematically investigate the correlation between magnetoresistance and structure symmetry. As the thickness of the SrRuO3 film increases, a structural symmetry transition from tetragonal to orthorhombic occurs. At the same time, a clear sign reversal of magnetoresistance from negative to positive, accompanied by the appearance of strong anisotropy in magnetoresistance measured along the two perpendicular in‐plane axes, is observed. These findings further suggest that the correlation between structural symmetry and magnetoresistance is mediated by the modulations in magnetic anisotropy. These results clarified the relationships between structure symmetry, magnetoresistance, and magnetic anisotropy, which can pave a feasible way for harnessing the magnetotransport properties of SrRuO3 films and using this material in oxide‐based spintronic devices. [ABSTRACT FROM AUTHOR]