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The formation and evolution of adiabatic shear behaviors, as well as the corresponding mechanical properties of a near-Ti-6Al-3Nb-2Zr-1Mo (Ti-6321) alloy during dynamic compression process, were systematically investigated by the split Hopkinson pressure bar (SHPB) compression tests in this paper. Ti-6321 samples containing three types of microstructures, i.e., equiaxed microstructure, duplex microstructure and Widmanstätten microstructure, were prepared to investigate the relationship between microstructures and dynamic mechanical behaviors under different strain rates in a range from 1000 s−1 to 3000 s−1. It was found by the dynamic strain–stress relation that the Ti-6321 alloys containing equiaxed microstructure, duplex microstructure and Widmanstätten microstructure all exhibited a strong strain-hardening effect. The samples containing equiaxed microstructure exhibited a larger flow stress than samples containing duplex microstructure and Widmanstätten microstructure. The adiabatic shearing behaviors in Ti-6321 alloy are significantly influenced by different types of microstructures. The formation of adiabatic shearing bands occurs in equiaxed microstructure when the strain rate is increased to 2000 s−1. The adiabatic shear bands are formed in duplex microstructure when the strain rate reaches 3000 s−1. However, the initiation of adiabatic shear bands is found in Widmanstätten microstructure under the strain rate of 1000 s−1. The Widmanstätten microstructure shows a larger sensitivity to adiabatic shearing than the equiaxed microstructure and duplex microstructure samples.