The preparation and the characterization of intercalation compounds of Mg–Al layered double hydroxide (Mg–Al LDH) and various organic surfactants have been studied in detail. The preparation has been carried out following regeneration method. The aim of such organic modification is to prepare LDHs suitable for application in polymer-LDH nanocomposites. The LDH-surfactant hybrids have been characterized by wide angle X-ray scattering (WAXS) and Fourier transform infrared (FTIR) spectroscopy. The modified Mg–Al LDH materials show an increase in interlayer distance as compared to the unmodified Mg–Al LDH depending on the length of the surfactant anions. Thermal decomposition changed significantly after organic modification. The particle morphology was investigated by scanning electron microscopy (SEM).