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Layered double hydroxide (LDH) is a promising flame-retardant nano-additive for polymers, however, its efficiency is highly based on its composition and dispersity. Based on this cognition, a core-shell LDH-based architecture (LDH@TA-HP) was designed using LDH sheet as core and tannic acid and phosphazene cross-linkd polymers network (TA-HP) as shell. In the flame retardant process, renewable tannic acid (TA) as a carbon source with phosphazene was combined to form an intumescent flame-retardant system, which synergizes with the "tortuous path" effect of LDH which greatly enhance the flame retardancy of PP and LDH@TA-HP composites (PP/LDH@TA-HP). With the addition of 20 wt% LDH@TA-HP, the peak heat release rate and total smoke production of the PP/LDH@TA-HP composites were decreased by 63.5% and 47.6%, respectively, in comparison with those of Neat PP. The flame retardant level reached UL-94 V-0 rating and the limiting oxygen index (LOI) value of PP/LDH@TA-HP composites reached 30.1%, which was related to the "tortuous path" effect of LDH and the formation of the intumescent char layer of TA-HP. This investigation provided a facile strategy for the design of multifunctional LDH-based hybrids, expanding LDH potential applications in polymer composites. [Display omitted] • A novel core-shell LDH-based flame retardant was prepared via a facile method. • LOI value of 20 wt% PP/LDH@TA-HP reached 30.1% and passed UL-94 V-0 rating. • TA-HP obviously enhanced the interaction between LDH@TA-HP and PP matrix. [ABSTRACT FROM AUTHOR]