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In this paper, a Phosphorous ‐ Aluminium ‐ Nitride synergistic flame retardant (PAN) was synthesized by phosphoric acid, glycerol, aluminium sulfate and urea, though a one‐pot process. The PAN was durably grafted onto the surface of cotton fabric by the simple process of soak‐dry‐cure. At the same time, the synergistic effect of the aluminium element and Phosphorous ‐ Nitrogen flame retardants (PN) was investigated. The flame‐retardant effect is the best when the conttent of alumium is 2.5 mol% (percentage of phosphoricacid) in PAN. The analyses of FTIR and XPS results suggested that PAN was grafted onto the cotton by forming a strong P−O‐C covalent bond on the surface of fiber. The SEM and Whiteness test proved that the flame‐retardant finishing cotton fabric do possess good morphology and whiteness. The thermal stability and flame retardancy of the PAN treated cotton fabric were assessed by TG and vertical flammability test. Then, found the aluminium sulfate in PAN had synergistic effect, and the PAN had significant flame retardancy in application.