The present research discussed the utilization of layered double hydroxides (LDH) materialswith different morphologies as adsorbents for Methyl Orange (MO) removal from aqueous solution. The adsorption properties of LDH with flower-like morphology (f-LDH) have been investigated for azo dye, Methyl Orange (MO), and compared to conventional stone-like coprecipitated LDH phases (c-LDH). Flower-like LDH with high specific surface area of 133m2/g were synthesized by coprecipitationmethod in dilute alkaline solution.With relatively high specific surface areas, the as-prepared flower-like LDH, when tested as adsorbents in azo dye removal, showed excellent performance and were better than those of conventional coprecipitated LDH. The adsorption isotherms, kinetics and mechanisms for azo dyeMO onto as-prepared flower-like LDH were also investigated. The high uptake capability of the as-prepared flower-like adsorbents 500.6 mg ofMO/g of LDH make thempotentially attractive adsorbents in water purification avoiding calcination step. Hence, a low cost material will be acquired with much more benefits namely preserving energy.