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LT21 a type of aluminum alloy used for the irradiation channel of the first heavy water research reactor (HWRR) in China. Studying the mechanical property of irradiated LT21 aluminum under actual service conditions is essential for evaluating its application property. In this paper, tensile specimens of irradiated LT21 were manufactured from the decommissioned irradiation channel of an HWRR; then, tensile tests were carried out, and then the fracture surfaces were observed. The effect of neutron irradiation on tensile behavior and the failure mechanism was analyzed by comparing the result of irradiated and unirradiated LT21 specimens. The results show that, with the thermal neutron flux increasing to 2.38 × 1022 n/cm2, the YS gradually increased from the initial 158 MPa to 251 MPa, the UTS increased from 262 MPa to 321 MPa, and the elongation decreased from 28.8% to about 14.3%; the brittle fracture of the LT21 specimen appeared after irradiation, and the proportion of brittle fracture increased as the neutron fluence increased; the nanophase structures, with a size of less than 50 nm, were precipitated in the LT21 aluminum alloy after neutron irradiation. Transmutation Si is presumed to be the main cause of the radiation effect mechanism of LT21. [ABSTRACT FROM AUTHOR]