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Three organophosphorus compounds, N-hydroxymethyl-3-dimethylphosphonopropionamide (HDPP), triallyl phosphate (TAP) and triallyl phosphoramide were employed in a study on flame retardant (FR) mechanisms. N-hydroxymethyl-3-dimethylphosphonopropionamide was more efficient in providing flame retardancy to cellulosic fabrics at the same phosphorus content on cotton fabrics. The flame retardance of the flame retardant treated cotton fabrics were characterized by using limiting oxygen index (LOI). Structural changes of the treated cotton fabrics and the compounds were carried out by using thermal analysis methods such as differential scanning calorimeter (DSC) and thermal gravimetric analysis and Fourier transform infrared (FTIR) spectroscopy. A new mechanism was proposed based on the efficient flame retardant performance of N-hydroxymethyl-3-dimethylphosphonopropionamide.