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In this work, using ferroferric oxide (Fe3O4) and zirconium oxide (ZrO2) as laser-sensitive particles and thermoplastic polyurethane (TPU) as the matrix resin, a series of TPU/Fe3O4/ZrO2 composites were prepared by melt blending, and the effect of the laser marking additive content, composition, and laser marking parameters on the laser marking properties of composites was investigated. The laser marking mechanism of Fe3O4/ZrO2 additives and the role of each component in TPU laser marking were studied by metallographic microscopy, color difference test, scanning electron microscopy, and Raman spectroscopy. Fe3O4 nanoparticles as a laser sensitizer component, on the one hand, can act as a pigment to make the TPU substrate black and, on the other hand, can absorb laser energy to contribute to the formation of laser markings on TPU composite surfaces. In addition, the introduction of ZrO2 nanoparticles can help absorb the laser energy, while the contrast can be improved to enhance the laser marking performance of the TPU composite. Through thermogravimetric analysis, the changes in the thermally stable properties of TPU composites before and after laser marking were investigated, and the results indicated that Fe3O4/ZrO2nanoparticles can absorb the laser energy, causing melting and pyrolysis of the TPU backbone at a high temperature, to produce a gaseous product resulting in foaming. Finally, the high-contrast and light-colored markings were formed on the black TPU composite surface. This work provides a facile method for producing high-contrast and light-colored markings on the dark TPU