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In this article, carbon microspheres (CMSs) synthesized by the hydrothermal method and CMSs-Fe (with Fe3+ adsorbed on the surface of CMSs) were combined with ammonium polyphosphate (APP) to achieve the fire safety improvement of thermoplastic polyurethane (TPU). The fire safety performance of TPU composites was investigated by the cone calorimeter test, microscale combustion calorimeter test, thermogravimetric analysis/infrared spectrometry, Raman spectrometry, X-ray photoelectron spectroscopy, and scanning electr