Complex oxides such as perovskite cobaltites exhibit rich phenomena at interfaces due to the complex interplay between their structural, defect, electronic, and magnetic degrees of freedom. We study this interplay here in the ferromagnetic metallic cobaltite ${\mathrm{La}}_{1\text{−}x}{\mathrm{Sr}}_x{\mathrm{CoO}}_{3\text{−}\delta }$, using specific substrates to vary both the heteroepitaxial strain (compressive $\mathrm{vs}$ tensile) and growth orientation ((001) $\mathrm{vs}$ (110)). Transmission electron microscopy, electron energy-loss spectroscopy, high-resolution X-ray diffraction, magnetometry, polarized neutron reflectometry, and electronic magnetotransport measurements are applied. Lattice mismatch and growth orientation are found to enable the precise control of interfacial oxygen vacancy ordering in ${\mathrm{La}}_{1\text{−}x}{\mathrm{Sr}}_x{\mathrm{CoO}}_{3\text{−}\delta }$, thus dictating strain relaxation and oxygen vacancy depth profiles, in turn controlling thickness-dependent magnetic and electronic properties. In particular, compressive strain and (110) orientations minimize deleterious magnetic/electronic dead layer effects, leading to the optimization of interfacial magnetism and transport. Strain and orientation tuning of oxygen vacancy ordering are thus established as powerful means to control physical properties at cobaltite-based interfaces, relevant to several fields.

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• Defects
• Electrical properties
• Magnetism
• Complex oxides
• Interfaces