To stabilize the fragrances with high volatility and chemical instability, various carriers or matrix have been employed to encapsulate the fragrance molecules. However, it is still a challenge to acquire high-loading and long-lasting fragrances due to the complicated reaction procedure or the lack of the efficient interactions between the matrix and fragrances. Herein, we have introduced layered double hydroxides (LDHs) to localize the fragrant vanillin molecules through the electrostatic interaction and hydrogen bonds between aldehyde group of vanillin and hydroxyl groups on the LDHs, and the loading contents of vanillin in the composites reached 1208 mg/g. The as-prepared composites showed high stability, and the fragrance retention ability of vanillin was significantly promoted in a long-term preservation due to the stabilization of LDHs. Moreover, the fragrant vanillin in the composites could be sustainably released upon the thermal treatment. Therefore, we have provided a long-lasting fragrant composite by encapsulating the fragrances into the inorganic LDHs through electrostatic interaction and hydrogen bonds, and it is anticipated that this strategy could provide insights into stabilization and controlled release of fragrances.