To date, many nanoadsorbents have been developed and used to eliminate heavy metal contamination, however, one of the challenges ahead is the preparation of adsorbents from processes in which toxic organic solvents are used in the least possible amount. Herein, we have developed a new carboxylic acid-functionalized layered double hydroxide/metal–organic framework nanocomposite (LDH/MOF NC) using a simple, effective, and green in situ method. UiO-66-(Zr)-(COOH)₂ MOF nanocrystals were grown uniformly over the whole surface of COOH-functionalized Ni₅₀Co₅₀-LDH ultrathin nanosheets in a green water system under a normal solvothermal condition at 100 °C. The synthesized LDH/MOF NC was used as a potential adsorbent for removal of toxic Cd(II) and Pb(II) from water and the influence of important factors on the adsorption process was monitored. Various non-linear isotherm and kinetic models were used to find plausible mechanisms involved in the adsorption, and it was found that the Langmuir and pseudo-first-order models show the best agreement with isotherm and kinetic data, respectively. The calculated maximum adsorption capacities of Cd(II) and Pb(II) by the LDH/MOF NC were found to be 415.3 and 301.4 mg g⁻¹, respectively, based on the Langmuir model (pH = 5.0, adsorbent dose = 0.02 g, solution volume = 20 mL, contact time = 120 min, temperature = 25 ℃, shaking speed 200 rpm).