In this study, nanomuscovite adsorbents were prepared by intercalation with various organic intercalates (DTAB-TTAB-DTPA-PA-PN) and used to remove Cd2+and Pb2+from polluted water. The best nanomuscovite was prepared using DTPA and muscovite (Muc/DTPA) and characterized by XRD, TEM, EDX, FTIR, and BET surface area. The developed nanoadsorbent was used to remove Cd2+and Pb2+from polluted water. The effect of various factors, including contact time, adsorbent dosage, solution pH, and temperature, was investigated. The results reveal that the maximum adsorption of Cd2+and Pb2+was 91.5% and 97%, respectively, at the initial metal concentration 50 ppm, adsorbent dosage 0.2 g, contact time 60 min, solution temperature 25 °C, and pH 6 for Pb2+and pH 7 for Cd2+. Adsorption isotherm models (Freundlich, Langmuir, Dubunin–Radushkevich, and Temkin isotherm models) as well as kinetic models (pseudo-first-order, pseudo-second-order, Elovich, and intra-particle diffusion models) were employed to evaluate the experimental results. The adsorption of Cd2+and Pb2+on Muc/DTPA fitted well within the Langmuir isotherm model and followed pseudo-second-order kinetics. Thermodynamics parameters of metal adsorption indicated exothermic and spontaneous processes. Results were applied to the real wastewater that showed high Cd2+and Pb2+removal.