Nanocomposites containing magnetic iron oxide (magnetite) nanoparticles and layered double hydroxide (LDH) nanosheets were prepared by two different methods, exfoliation-reassembly and coprecipitation, for aqueous chromate adsorbent. According to X-ray diffraction, scanning electron microscopy, and atomic force microscopy, both nanocomposites were determined to develop different nanostructures; LDH nanosheets well covered magnetite nanoparticles with house-of-cards-like structure in exfoliation-reassembly method, while coprecipitation resulted in LDH particle formation along with magnetite nanoparticles. Zeta-potential measurement also revealed that the magnetite surface was effectively covered by LDH moiety in exfoliation-reassembly compared with coprecipitation. Time, pH, concentration dependent chromate adsorption tests, and magnetic separation experiments exhibited that both nanocomposites effectively adsorb and easily collect chromate. However, exfoliation-reassembly nanocomposite was determined to be slightly effective in chromate removal by ~10%. Chromate adsorbed nanocomposites could be regenerated by treating with bicarbonate and the regenerated nanocomposites preserved ~80% of chromate adsorption efficacy after three times of recycling.