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To address the increasing demand for lightweight, highly friction- and wear-resistant, integrally designed moving components in aerospace applications, this study systematically investigated the processability and wide-temperature-range properties of the MoS 2 /polyether-ether-ketone (PEEK) self-lubricating composites fabricated using the laser powder bed fusion (LPBF) process. The results demonstrated that the incorporation of MoS 2 enhanced powder flowability and thermal stability, albeit at the expense of laser absorptivity. Optimal processing parameters were established, achieving a porosity of less than 0.01%. Notably, adding MoS 2 significantly influenced the crystallization behaviour of PEEK, leading to tensile strengths exceeding 92 MPa at both room and low temperatures, along with an elongation greater than 20% at 150°C. The coefficient of friction for the 12 wt.% MoS 2 2 /PEEK self-lubricating composite was measured at 0.035, 0.11, and 0.058 at temperatures of −150, 20, and 150°C, respectively, representing a reduction of over 75% compared to pure PEEK. Correspondingly, the wear rates indicated a reduction of more than 80%. Additionally, the fracture and wear mechanisms of pure PEEK and the MoS /PEEK self-lubricating composites at extreme temperatures were revealed. This research lays a crucial foundation for the LPBF fabrication of self-lubricating polymer composites and advances their application within the aerospace industry.