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 Sr2IrO4 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 C4‐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.

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As one of the most fundamental physical phenomena, charge density wave (CDW) order predominantly occurs in metallic systems such as quasi‐one‐dimensional (quasi‐1D) metals, doped cuprates, and transition metal dichalcogenides, where it is well understood in terms of Fermi surface nesting and electron‐phonon coupling mechanisms. On the other hand, CDW phenomena in semiconducting systems, particularly at the low carrier concentration limit, are less common and feature intricate characteristics, which often necessitate the exploration of novel mechanisms, such as electron‐hole coupling or Mott physics, to explain. In this study, we combined electrical transport, synchrotron X‐ray diffraction and density‐functional theory (DFT) calculations to investigate CDW order and a series of hysteretic phase transitions in a dilute d‐band semiconductor, BaTiS3. Our experimental and theoretical findings suggest that the observed CDW order and phase transitions in BaTiS3 may be attributed to both electron‐phonon coupling and non‐negligible electron‐electron interactions in the system. Our work highlights BaTiS3 as a unique platform to explore CDW physics and novel electronic phases in the dilute filling limit and could open new opportunities for developing novel electronic devices.This article is protected by copyright. All rights reserved