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Wool and polyester blends are sensitive to heat and pose fire hazards. In this study, the flame retardancy of wool/polyester blended fabric was improved by coating montmorillonite (MMT) and polyquaternium-10 (PQ-10) using the layer-by-layer assembly (LBL) method. This was done to confirm the feasibility of combining eco-friendly materials such as MMT and PQ-10 coatings and to secure the flame retardancy of the wool/polyester blend. The phosphate-buffered solution enhanced the intermolecular forces during pretreatment. Scanning electron microscopy and Fourier-transform infrared spectroscopy analyses confirmed the successful deposition of the MMT/PQ-10 combination on the fabric, and the deposition on the fabric surface increased as the number of coating layers increased. The thermogravimetric analysis results showed that the MMT/PQ-10 combination effectively reduced the maximum decomposition temperature, contributing to improved high-temperature thermal stability. Additionally, compared with the untreated fabrics, the coated fabrics exhibited a 38.2% increase in residual substances, and flame-retardant properties enhanced up to 27.3%. As a result of the vertical flame test, the MMT/PQ-10 combination improves the cohesiveness of the fabrics and prevents melt dripping, contributing to the improvement of flame retardancy. [Display omitted] • Eco friendly flame-retardant coating was applied to wool/polyester fabric through Layer-by-Layer process. • The use of phosphate buffer improved interlayer bonding strength. • The combination of MMT/PQ-10 effectively improved the thermal stability of the fabric at high temperatures. • the coated fabrics exhibited a 38.2% increase in residual substances and flame-retardant properties enhanced up to 27.3%. • The melt drop phenomenon was eliminated from the treated fabrics. [ABSTRACT FROM AUTHOR]