The imidization mechanism, structure, and magnetic properties of organic modified Zinc-aluminum layered double hydroxides/polyimide composites are investigated. During imidization, organic modified Zinc-aluminum layered double hydroxides lose the hydroxyl group and sodium dodecyl sulfate modifier decomposes partly resulting in a loose contact between PI and oxidized Zinc-aluminum layered double hydroxides. The thermal properties of composites are slightly decreased with increasing organic modified Zinc-aluminum layered double hydroxides but the wettability varies oppositely. Comparing to organic modified Zinc-aluminum layered double hydroxides, the saturated magnetization of heated organic modified Zinc-aluminum layered double hydroxides is enhanced slightly due to structural improvement in Fe(3)O(4) crystalline domain. Therefore, the magnetic properties are not affected by imidization procedure. The soft magnetic composites have large potential in electromagnetic shielding.