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[Display omitted] • A multifunctional small molecule (HCPA) has been prepared. • The presence of HCPA endowed PVA with a nanostructure within the continuous matrix. • 5 wt% of HCPA endows PVA with a self-extinguishing behavior. • 5 wt% of HCPA increases tensile strength of PVA by 47% and toughness by 370%. • The PVA/HCPA composites exhibit a water-trigged healing efficiency over 90%. The combination of high fire retardancy, high strength, and great toughness as well as good healability is essential for successful real-world applications of polymeric materials in the fields of packaging, electronics & electrics, and optical devices. To date, there have been few successes in achieving such performance portfolios in polymers due to their different and even mutually exclusive governing mechanisms. Inspired by the nanoconfinement effect that governs the unique mechanical properties of spider silk, we, herein, rationally design a multifunctional small molecule, HCPA, that can serve as a fire retardant and hydrogen-bond crosslinker for poly(vinyl alcohol) (PVA). Benefiting from the dual-phase fire-retardancy effect and the dynamic cross-linking effect, the addition of 5.0 wt% of HCPA enables PVA to achieve a desired self-extinguishment in combination with a high tensile strength of 133 MPa and a toughness of 112 MJ/m3. In addition, the as-prepared polymer material exhibits a high healing efficiency of over 90% (based on strength) if triggered by water. This proof-of-concept opens numerous opportunities for the creation of self-extinguishing, strong, tough, and self-healing polymers for many high-end applications in the above-mentioned industries. [ABSTRACT FROM AUTHOR]

[Display omitted] • A multifunctional MXene-based hybrid (Zr-MXene) has been prepared. • 1 wt% of Zr-MXene increases ductility and toughness of TPU by 33% and 88%, respectively. • 1 wt% of Zr-MXene increases the tensile strength and fatigue resistance of TPU. • The addition of Zr-MXene significantly reduce the flammability of TPU. • The peak heat release rate and peak smoke production rate are respectively reduced by 63% and 56%. Thermoplastic polyurethane (TPU) features many important industrial applications, but intrinsic flammability extremely impedes its practical applications. Current fire-retardant strategies often lead to improved flame retardancy but reduced mechanical properties (strength, ductility, and toughness). Hence, to date it has been unsuccessful to design advanced TPU materials that are strong, stretchable, tough, fatigue-and fire-resistant to meet increasing performance portfolio requirements. Here, we report a hybridized fire retardant (Zr-MXene) by in situ facilely loading zirconium amino-tris-(methylenephosphonate) (Zr-AMP) onto the titanium carbide (MXene) surface. Our results show that with 1 wt% of Zr-MXene, the resultant TPU nanocomposites demonstrate a record break strain (2060%) and toughness (316 MJ/m3) to date, in addition to increased tensile strength by 43.4% and improved fatigue resistance relative to the TPU matrix, because of favorable interfacial hydrogen-bonding. Moreover, the resultant TPU material exhibit significantly reduced flammability as a result of the combined physical barrier, catalytical carbonization and diluting effects of Zr-MXene. This work provides a promising strategy for the creation of multifunctional MXene and its polymeric nanocomposites, which hold great promise for many industrial applications. [ABSTRACT FROM AUTHOR]