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The gradient nanocrystalline structure from the topmost surface to the matrix of a bulk coarse-grained TC17 was attained by using high energy shot peening treatment at an air pressure of 0.35 MPa and a processing duration of 30 min. The thickness from the topmost surface with a grain size of about 10.5 nm to the matrix with a micrometer structure was about 120 μm, and the thickness in the nanocrystalline layer was about 20 μm. The microscopic and nanocrystalline structure characteristic in the treated layer were investigated via X-ray diffraction, scanning electron microscopy and high-resolution transmission electron microscopy. The nanograins layer, the nanometer-thick laminated structure layer, the refined grains layer and the low-strain matrix layer occurred in sequence from the topmost surface to the matrix, and therefore the gradient nanocrystalline structure in the treated layer was produced by using high …