Cadmium telluride (CdTe) is a highly promising material for photovoltaics (PV) and photodetectors due to its light‐absorbing properties. However, efficient design and use of flexible devices require a deep understanding of its atomic‐level deformation mechanism. Herein, uniaxial compression deformation of CdTe monocrystalline with varying crystal orientations is investigated using molecular dynamics (MD) with a newly developed machine‐learning force field (ML‐FF), alongside in‐situ micropillar compression experiments. The findings reveal that CdTe bulk deformation is dominated by reversible martensitic phase transformation, whereas CdTe pillar deformation is primarily driven by dislocation nucleation and movement. CdTe monocrystals possess exceptional super‐recoverable deformation along the <100> orientation due to hyper‐elastic processes induced by martensitic transformation. This discovery not only sheds light on the peculiarities observed in micropillar experimental measurements, but also provides pivotal insights into the fundamental deformation behaviors of CdTe and similar II–VI compounds under various stress conditions. These insights are crucial for the innovative design and enhanced functionality of future flexible electronic devices.
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