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Protective textiles have been the primary choice in protecting humans from hazardous substances. Conventional protective textiles are shifting towards a smart and sustainable alliance. Nanomaterials are emerging materials that can be incorporated into traditional fabrics for the development of advanced smart and sustainable protective textiles due to their enhanced mechanical/chemical properties, high catalytic and disinfection efficiency, flame retardance and photoprotection capabilities. Recent literature shows that the addition of various nanomaterial-based fillers, including nanoparticles and electrospun nanofibres, can significantly promote multifunctionality. Therefore, this chapter highlights the potential and challenges faced by nanomaterial-based protective textiles in building a smart and sustainable protective textiles society for the future.