A poly(methyl acrylate)(PMA)/ZnAl layered double hydroxide(ZnAl-LDH) intercalation nanocomposite is synthesized by in situ polymerization of methyl acrylate with ogano-modified ZnAl-LDH(O-ZnAl-LDH). Its structure and morphology are confirmed by X-ray diffraction(XRD) and transmission electron microscopy(TEM) image. The d 001 of O-ZnAl-LDH is expanded to 2.85 nm after polymerization from 2.63 nm, which indicates the intercalation of PMA chains into the galleries of O-ZnAl-LDH. The (001) diffraction of PMA/ZnAl-LDH nanocomposite is broad due to the exfoliation of some O-ZnAl-LDH layers. The TEM image shows that the most of the layers of O-ZnAl-LDH are stacked with a distance of about 3 nm while some of them are exfoliated and dispersed disorderly in the PMA matrix.