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Expanding the application range of flame-retardant polymer biocomposites remains a huge challenge for a sustainable society. Despite largely enhanced flame retardancy, until now the resultant poly(lactic acid) (PLA) composites still suffer reduced tensile strength and impact toughness due to improper material design strategies. We, herein, demonstrate the design of a green flame retardant additive (ammonium polyphosphate (APP)@cellulose nanofiber (CNF)) via using the cellulose nanofibers (CNFs) as the green multifunctional additives hybridized with ammonium polyphosphate (APP). The results show that PLA composite with 5 wt % loading of APP@CNF can pass the UL-94 V-0 rating, besides a high limited oxygen index of 27.5%, indicative of a significantly enhanced flame retardancy. Moreover, the 5 wt % of APP@CNF enables the impact strength (σ i ) of the PVA matrix to significantly improve from 7.63 to 11.8 kJ/m 2 (increase by 54%), in addition to a high tensile strength of 50.3 MPa for the resultant flame-retardant PLA composite. The enhanced flame retardancy and mechanical strength performances are attributed to the improved dispersion of APP@CNF and its smaller phase size within the PLA matrix along with their synergistic effect between APP and CNF. This work opens up a facile innovative methodology for the design of high-performance ecofriendly flame retardants and their advanced polymeric composites.

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