Novel modified Ni/Fe layered double hydroxides with different morphology of spherical-like shape were fabricated via using urea as a ligand and glycerol (Ni/Fe LDH/GL) with Ni:Fe molar ratios of 2:1 by the simplest co-precipitation method. Also, for comparison purposes, Ni/Fe LDH was synthesized to be used as a control one. A suggested interpretation for the morphology change was also given. The materials were characterized by X-ray diffraction (XRD), The Fourier transform infrared (FT-IR) spectroscopy, field emission scanning electron microscopy (FESEM), EDX for elemental analysis, high resolution transmission electron microscopy (HRTEM), Brunauer, Emmett, and Teller (BET) equation, particle size distributions and Zeta potential measurements. In addition, the synthesized materials were used as adsorbents for removal of potassium dichromate from aqueous solutions under various experimental conditions. The adsorption of Cr (VI) was strongly pH dependant and the pH PZC was studied. Kinetic studies were evaluated through different models including, pseudo first and second orders, mixed 1, 2 orders, intra particle diffusion and Avrami models. For adsorption isotherms, twoparameter models (Langmuir, Freundlich and Temkin) and three parameter models (Sips, Langmuir-Freundlich and Tooth) were investigated showing maximum adsorption capacity of 50.43 mg/g and 136.05 mg/g for Ni/Fe LDH and Ni/Fe LDH/GL, respectively. Also, the effect of temperature was investigated at (23, 35, 45, 55 °C) and the thermodynamic parameters (∆H°, ∆S° and ∆G°) were calculated showing exothermic and spontaneous adsorption process. The effect of coexisting anions (cl − , So 4 2− and HPO 4 2−) and humic acid at different concentrations on the removal efficiency of dichromate ions was investigated. Chemical stability and recyclability of these adsorbents were also studied. The intermolecular hydrogen bonds formation between dichromate ion, urea, glycerol, LDH was explored by Monte Carlo simulation This study suggested that the modified Ni/Fe LDH/GL materials were promising nanoadsorbents for efficient potassium dichromate removal. Water is the most precious natural source important for human beings, agriculture, and industrial activities. Recently, water bodies are potentially contaminated and polluted by many hazardous materials such as nuclear and industrial wastes, pharmaceuticals, organic contaminants and heavy metals. Heavy metals like cadmium, zinc, copper, lead, arsenic, mercury and chromium have significant threat to human health due to its potentially toxic effects 1,2. Chromium is one of heavy metals widely used in many industrial processes such as electroplating, dyes, mining, photography, textile and leather 3. Chromium present in water in a trivalent and hexavalent oxidation state, it is established that hexavalent chromium exhibits high toxicity toward living organisms than trivalent chromium which in contrast is a micronutrient 4. Hexavalent chromium is reported as a cause of respiratory cancers 5,6 and mutations and chromosomal dam...