Abstract: Uranium is used as a fuel for nuclear power plant and can be extracted from different ores, mainly acidic (silicious ore) and alkaline (carbonate ore). Recovery of uranium through acid leaching from silicious ore is well established, whereas, alkaline leaching from carbonate ore is challenging due to the excessive salinity of leach liquor and high concentration of carbonate, bicarbonate and sulphate. Herein, two monomers, acrylic acid (AA) and N, N-methylene bisacrylamide (BAM), selective towards uranyl were intercalated in-situ into the interlayer, followed by their polymerization and cross-linking to form novel polymer intercalated hybrid layered double hydroxide (LDH). The LDH acts as a backbone to overcome coiling and swelling of polymer and anchors them as free-standing. Various parameters, like, the type of metal ions, monomer ratio (AA: BAM) and metal ion ratio (M2+:M3+), were studied to determine the optimum conditions for effective intercalation and polymerization of monomers. Magnesium aluminum (MgAl) LDH with a cross-linked polymer having a monomer ratio of 3:2 (AA: BAM) as intercalating species showed maximum efficiency of uranyl adsorption (1456 mg/g at 30 °C) with highest capacity so far. The distribution coefficient (Kd, l/mg) in the order of 105 suggested that the adsorbent was highly selective for uranyl in the presence of different cations, anions and humic acid. The adsorbent extracts uranium effectively and selectively from a real-life alkaline leach liquor with an efficiency of 96% at 5 g/l dose. Uranium can be recovered from the adsorbent in the form of sodium di-uranate using 2(M) NaOH and was reused for eight cycles.