In this study Mg/Al-layered double hydroxide (LDH) was intercalated with diacid containing L-aspartic acid in one step using ultrasonic method under green conditions. Organic diacid was used as modifier to enhance their compatibility and led to better dispersion of LDH nanoclay in polymer matrix. An effective intercalation of the examined diacid in LDH was confirmed by several techniques such as Fourier transform-infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), X-ray diffraction (XRD), field emission-scanning electron microscopy (FE-SEM) and transmission electron microscopy (TEM). Then, novel optically active poly (amide-imide)/modified LDH nanocomposites (PAI/M-LDH NCs) containing L-phenylalanine moiety were successfully synthesized via a green and inexpensive ultrasonic irradiation process. For this purpose at the first, PAI was employed as polymer matrix and was synthesized by direct poly condensation reaction of N,N -(pyromellitoyl)-bis- L -phenylalanine with 4,4-diamino diphenyl sulfone in molten tetra-n-butyl ammonium bromide as solvent and triphenyl phosphite as a green condensing agents. TGA data indicated an improvement in thermal stability of the polymer NCs compared to the pure polymer. FE-SEM and TEM images of NCs showed that the M-LDH nanoclay are uniformly dispersed on the surface of PAI matrix. In the second study, poly (vinyl alcohol) (PVA)/M-LDH NCs were successfully synthesized via a simple and inexpensive ultrasonic irradiation process. TGA analysis showed an improvement in thermal stability of the polymer NCs compared to the pure PVA and FE-SEM images of NCs showed that the M-LDH nanoclay are homogenously dispersed on the surface of PVA matrix. Tensile strength and modulus improved for PVA/M-LDH NCs in comprising of the pure PVA. Enhancement in the mechanical properties results from hydrogen bonding and the well dispersion of the M-LDH in the polymer matrix.