This paper presents the synthesis of an accordion-like structural Ti₃C₂@CuS material with copper sulfide nanospheres firmly anchored on the Ti₃C₂Tx surface using the hydrothermal method. The resulting few-layered nanosheets exhibit good dispersion in polyurethane (PU) and exhibit excellent mechanical and thermal stability due to coordination bonding between PU and the released Cu2+. Ti₃C₂@CuS-PU also demonstrates a highly effective self-healing performance and long-term sterilization ability, thanks to the synergistic effect of sustained copper ion release, elevated ROS production, and excellent Ti₃C₂@CuS dispersion in PU. This work offers a promising pathway to creating multifunctional antibacterial self-healing materials.