Herein, we have synthesized a microspherical nickel‐cobalt‐layered double hydroxides‐reduced graphene oxide composite (NiCo‐LDHs‐rGO) through a one‐step hydrothermal method and then used it as an adsorbent for the removal of Pb2+ from aqueous solutions. Fourier transform infrared spectrophotometry (FT‐IR), field emission scanning electron microscopy (FESEM), mapping elemental analysis, electron dispersive x‐ray spectroscopy (EDX), x‐ray diffraction analysis (XRD), and the Brunauer–Emmett–Teller (BET) method were used for the characterization of the adsorbent. Factors affecting the adsorption of Pb2+ ion such as solution pH, adsorbent dosage, contact time, competing ion, and regeneration were investigated in batch mode by the NiCo‐LDHs‐rGO. Under optimized conditions based on the Taguchi method (pH = 5.0, adsorbent dosage = 20 mg, and contact time = 30 min), the highest removal percentage was found to be 99.7% for 100 mg L−1 of Pb2+. According to the results, NiCo‐LDHs‐rGO exhibited a high preference for Pb2+ over Cu2+, Zn2+, and Cd2+. This adsorbent was regenerated for several cycles (using 0.01 M HCl) with no significant deterioration in performance. Analyses of the adsorption isotherm models revealed that the adsorption of Pb2+ follows Freundlich isotherm with a maximum adsorption capacity of 200 mg g−1. Also, the kinetic data confirmed that pseudo second order kinetic equation is the best model for predicting the kinetics. Furthermore, the Simulink modelling illustrated that the adsorption kinetics of Pb2+ onto NiCo‐LDHs‐rGO is done with high accuracy in a continuous stirred‐tank reactor. Finally, dual interactions of the effective parameters can be modelled by polynomial equations in MATLAB, and according to the Taguchi model, pH is clearly the most important feature among all effective parameters.