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Effective nonmagnetic control of the spin structure is at the forefront of the study for functional quantum materials. This study demonstrates that, by applying an anisotropic strain up to only 0.05%, the metamagnetic transition field of spin–orbit‐coupled Mott insulator Sr 2 IrO 4  can be in situ modulated by almost 300%. Simultaneous measurements of resonant X‐ray scattering and transport reveal that this drastic response originates from the complete strain‐tuning of the transition between the spin‐flop and spin‐flip limits, and is always accompanied by large elastoconductance and magnetoconductance. This enables electrically controllable and electronically detectable metamagnetic switching, despite the antiferromagnetic insulating state. The obtained strain‐magnetic field phase diagram reveals that C 4 ‐symmetry‐breaking anisotropy is introduced by strain via pseudospin‐lattice coupling, directly demonstrating the pseudo‐Jahn–Teller effect of spin–orbit‐coupled complex oxides. The extracted coupling strength is much weaker than the superexchange interactions, yet crucial for the spontaneous symmetry‐breaking, affording the remarkably efficient strain‐control.

Comprehensive Electrical Control of Metamagnetic Transition of a Quasi‐2D Antiferromagnet by In Situ Anisotropic Strain