We investigated the selective deoxyribonucleic acid (DNA) adsorption on layered double hydroxide (LDH) nanoparticles via studying the interaction between positively charged LDH nanoparticle as adsorbent and negatively charged adsorbates such as methyl orange (MO), fluorescein (FL), and DNA strands. The size controlled LDH (Mg 0.78Al 0.22(OH) 2(CO 3) 0.11 · mH 2O) was prepared by conventional coprecipitation method, followed by the hydrothermal treatment. According to the adsorption isotherms, the adsorbed amounts of MO and FL were similar, however, that of DNA were much larger. The adsorption behaviors were well fitted to Freundlich adsorption model. The concentration dependent adsorption behavior on LDH surface was described in order to verify the selective DNA separation ability. The result showed that the LDH has advantages in selective adsorption of DNA competing with single molecular anions.