Rosette-like layered double hydroxide (roseLDH) crystals with interlayer CO 3 2− anions were synthesized by the reaction of Mg(NO 3 ) 2 , Al(NO 3 ) 3 , and hexamethylenetetramine (HMT) at 140 °C over 4 days. Crystals as large as 20 μm were produced when using a specific range of HMT concentrations. The substitution of CO 3 2− interlayer ions with ClO 4 − or Cl − anions was achieved by the addition of perchloric acid or hydrochloric acid, respectively, to dispersion of material in methanol. The products were denoted as CO 3 2− roseLDH, ClO 4 − roseLDH, and Cl − roseLDH, respectively. These LDHs were characterized using X-ray diffraction under controlled relative humidity, as well as by Fourier transform infrared spectroscopy and scanning electron microscopy. Adsorption experiment with anions such as phosphate (HPO 4 2− ) and nitrate (NO 3
−) was conducted by using ClO 4 − roseLDH and Cl − roseLDH. The results indicate that both anions were adsorbed through an ion-exchange mechanism. The maximum HPO 4 2− adsorption capacity at equilibrium on ClO 4 − roseLDH was 1.6 mmol g −1 (49.6 mg P g −1 ), which corresponds to approximately 75% of the total positive layer charge. Cl − roseLDH showed a similar adsorption capability. Commercially available platelike LDH particles were essentially impermeable to water flow due to clogging, while the roseLDH crystals showed excellent permeability, an order of magnitude higher than that exhibited by the platelike LDH synthesized using a homogeneous precipitation method with different growth conditions. Anion adsorption during batch and flow-through test with the ClO 4 − roseLDH (mean particle diameter ∼ 38 μm) in a packed bed showed good uptake of HPO 4 2− and NO 3 − from aqueous solutions. These results demonstrate the potential of roseLDH materials to serve as a column filler adsorbent of the hazardous anions.