Well-defined finite particles of nitrate forms of layered double hydroxides (MgAl and NiAl types) were successfully synthesized from aqueous solution of metal nitrates by the recently developed pH adjustment method, where hydroxide form ion exchange resin was used to change a starting acidic solution into basic solution for the hydroxide formation. The interlayer nitrate ion of layered double hydroxide was exchanged with such anions as dodecylsulfate and oleate to form intercalation compounds by conventional anion exchange reactions in aqueous media at room temperature, suggesting potential of the methods as well as the present materials for further study on the applications of LDHs.