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Deterministic tuning of domain populations has typically remained limited to local solutions, or removal with temperature. Here, the manipulation of ferroelastic domain structure, and removal of the twin walls between them in single\u2010crystal  using in situ uniaxial strain is demonstrated. Combining atomic force microscopy, X\u2010ray diffraction, and Raman spectroscopy with first\u2010principles calculations, the microscopic evolution of the twin domain population is mapped through a strain\u2010driven transition from the rhombohedral  ground state toward the predicted orthorhombic  phase. Applied strains below  produce pronounced surface flattening and large\u2010scale domain reorganization, establishing uniaxial strain as a technically accessible tuning parameter for ferroelastic domain engineering. 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