Polyethylene is used as a traditional shielding material in the nuclear industry, but still suffers from low softening point, poor mechanical properties, and difficult machining. In this study, novel boron carbide polyether-ether-ketone (PEEK) composites with different mass ratios were prepared and tested as fast neutron absorbers. Next, shielding test pieces with low porosity were rapidly manufactured through the fused deposition modeling (FDM)-3D printing optimization process. The respective heat resistances, mechanical properties, and neutron shielding characteristics of as-obtained PEEK and boron carbide PEEK composites with different thicknesses were then evaluated. At load of 0.45 MPa, the heat deformation temperature of boron carbide PEEK increased with the boron carbide content. The heat deformation temperature of 30% wt. boron carbide PEEK was recorded as 308.4 °C. After heat treatment, both tensile strength and flexural strength of PEEK and PEEK composites rose by 40%–50% and 65%–78%, respectively. Moreover, the as-prepared composites showed excellent fast neutron shielding performances. For shielding test pieces with thicknesses between 40 mm and 100 mm, the neutron shielding rates exhibited exponential variation as a function of boron carbide content. The addition of 5%–15% boron carbide significantly changed the curvature of the shielding rate curve, suggesting an optimal amount of boron carbide. Meanwhile, the integrated shielding/structure may effectively shield neutron radiation, thereby ensuring optimal shielding performances. In sum, further optimization of the proposed process could achieve lightweight materials with less consumables and small volume.
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