The rare-earth orthoferrite family is prototypical strongly correlated systems, known for its highly tunable ferromagnetism properties. Among these materials, $\mathrm{S}{\mathrm{m}}_{0.5}{\mathrm{Y}}_{0.5}\mathrm{Fe}{\mathrm{O}}_3$ exhibits potential for applications becaue of its near room temperature spin reorientation transition. However, a comprehensive understanding of the spin reorientation and structural phase transitions in $\mathrm{S}{\mathrm{m}}_{0.5}{\mathrm{Y}}_{0.5}\mathrm{Fe}{\mathrm{O}}_3$ under pressure remains unclear. In this work, we present spectral (Raman and synchrotron x-ray diffraction) and electrical (electrochemical impedance spectroscopy) evidence of spin reorientation and an isostructural phase transition in $\mathrm{S}{\mathrm{m}}_{0.5}{\mathrm{Y}}_{0.5}\mathrm{Fe}{\mathrm{O}}_3$ up to 50 GPa. DFT calculations demonstrate that. while $\mathrm{S}{\mathrm{m}}_{0.5}{\mathrm{Y}}_{0.5}\mathrm{Fe}{\mathrm{O}}_3$ retains its semiconducting behavior under pressure, it undergoes a pressure-induced spin reorientation transition, with the magnetic easy axis switching from the (100) to the (001) direction. These findings establish pressure as a critical parameter for tuning correlated-electron behavior in $\mathrm{S}{\mathrm{m}}_{0.5}{\mathrm{Y}}_{0.5}\mathrm{Fe}{\mathrm{O}}_3$, paving the way for applications in spintronic and next-generation quantum transportation devices.

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• Pressure effects
• Rare-earth magnetic materials
• Density functional calculations
• Raman spectroscopy
• X-ray diffraction