We have hybridized Angelic gigas Nakai flower extract (AGNF) and two-dimensional layered double hydroxide (LDH) nanomaterials through reversible dehydration-hydration in order to obtain the nanopowder of natural extract. The Angelica gigas Nakai flower was treated with methanol to extract carbohydrate, polyphenol, and flavonoid components. LDH with an uniform size of 250 nm was prepared by hydrothermal method and calcined at 400ºC to obtain layered double oxide (LDO) precursor. For hybridization, AGNF in 40% methanol was reacted with LDO powder at various AGNF/LDO weight ratios: 0.15, 0.30, 0.85, and 1.70. The hybrids were obtained in fine powder which had enhanced hydrophilicity and water dispersity compared with dried AGNF. The X-ray diffraction and scanning electron microscopic results revealed that the house-of-cards structure of nanomaterials could encapsulate AGNF moiety inside their cavity. Quantitative analyses using UV-Vis spectra exhibited that the content of AGNF in hybrid increased upon AGNF/LDO ratio in reactant increased. According to 1,1-diphenyl-2-picrylhydrazyl radical scavenging assay, AGNF/LDO showed higher antioxidant activity compared with an equivalent amount of AGNF itself.