Pb(ii) adsorption by MnO2/MgFe-layered double hydroxide (MnO2/MgFe-LDH) and MnO2/MgFe-layered metal oxide (MnO2/MgFe-LDO) materials was experimentally studied in lab-scale batches for remediation property and mechanism analysis. Based on our results, the optimum adsorption capacity for Pb(ii) was achieved at the calcination temperature of 400 °C for MnO2/MgFe-LDH. Langmuir and Freundlich adsorption isotherm models, pseudo-first-order and pseudo-second-order kinetics, Elovich model, and thermodynamic studies were used for exploring the Pb(ii) adsorption mechanism of the two composites. In contrast to MnO2/MgFe-LDH, MnO2/MgFe-LDO400 °C has a stronger adsorption capacity and the Freundlich adsorption isotherm model (R2 > 0.948), the pseudo-second-order kinetic model (R2 > 0.998), and the Elovich model (R2 > 0.950) provide great fits to the experimental data, indicating that the adsorption occurs predominantly via chemisorption. The thermodynamic model suggests that MnO2/MgFe-LDO400 °C is spontaneously heat-absorbing during the adsorption process. The maximum adsorption capacity of MnO2/MgFe-LDO400 °C for Pb(ii) was 531.86 mg g-1 at a dosage of 1.0 g L-1, pH of 5.0, and temperature of 25 °C. Through characterization analysis, the main mechanisms involved in the adsorption process were precipitation action, complexation with functional groups, electrostatic attraction, cation exchange and isomorphic replacement, and memory effect. Besides, MnO2/MgFe-LDO400 °C has excellent regeneration ability in five adsorption/desorption experiments. The above results highlight the powerful adsorption capacity of MnO2/MgFe-LDO400 °C and may inspire the development of new types of nanostructured adsorbents for wastewater remediation.