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In this paper, we report an in situ study regarding the microstructural evolution of a Cr20Ni80 alloy with high proportional twin boundaries by using electron backscatter diffraction techniques combined with the uniaxial tensile test. The study mainly focuses on the evolution of substructure, geometrically necessary dislocation, multiple types of grain boundaries (especially twin boundaries), and grain orientation. The results show that the Cr20Ni80 alloy can be obtained with up to 73% twin boundaries by annealing at 1100 °C for 30 min. During this deformation, dislocations preferentially accumulate near the twin boundary, and the strain also localizes at the twin boundary. With the increasing strain, dislocation interaction with grain boundaries leads to a decreasing trend of twin boundaries. However, when the strain is 0.024, the twin boundary is found to increase slightly. Meanwhile, the grain orientation gradually rotates to a stable direction and forms a Copper, S texture, and α-fiber <110>. Above all, during this deformation process, the alloy is deformed mainly by two deformation mechanisms: mechanical twinning and dislocation slip.

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