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This study investigates the microstructures and deformation mechanism of hetero-structured pure Ti under different high strain rates (500 s⁻¹, 1000 s⁻¹, 2000 s⁻¹). It has been observed that, in samples subjected to deformation, the changes in texture are minimal and the rise in temperature is relatively low. Therefore, the influence of these two factors on the deformation mechanism can be disregarded. As the strain rate increases, the dominance of dislocation slip decreases while deformation twinning becomes more prominent. Notably, at a strain rate of 2000 s⁻¹, nanoscale twin lamellae are activated within the grain with a size of 500 nm, which is a rarely observed phenomenon in pure Ti. Additionally, martensitic phase transformation has also been identified. In order to establish a correlation between the stress required for twinning and the grain size, a modified Hall–Petch model is proposed, with the obtained value of <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msub><mi>K</mi><mrow><mi>t</mi><mi>w</mi><mi>i</mi><mi>n</mi></mrow></msub></mrow></semantics></math></inline-formula> serving as an effective metric for this relationship. These findings greatly enhance our understanding of the mechanical responses of Ti and broaden the potential applications of Ti in dynamic deformation scenarios.