In this work, the efficiency of the adsorptive removal of the organic cationic dye methylene blue (MB) from polluted water was examined using three materials: natural clay (zeolite), Zn-Fe layered double hydroxide (LDH), and zeolite/LDH composite. These materials were characterized via X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, high-resolution transmission electron microscopy (HRTEM), energy dispersive X-ray (EDX) diffraction (XRF), low-temperature N2 adsorption, pore volume and average pore size distribution and field emission scanning electron microscopy (FE-SEM). The properties of the applied nanomaterials regarding the adsorption of MB were investigated by determining various experimental parameters, such as the contact time, initial dye concentration, and solution pH. In addition, the adsorption isotherm model was estimated using the Langmuir, Freundlich, and Langmuir–Freundlich isotherm models. The Langmuir model was the best-fitting for all applied nanomaterials. In addition, the kinetics were analyzed by using pseudo-first-order, pseudo-second-order, and intraparticle diffusion models, and the pseudo-second-order model was an apparent fit for all three applied nanomaterials. The maximum Adsorption capacity toward MB obtained from the materials was in the order zeolite/LDH composite > zeolites > Zn-Fe LDH. Thus, the zeolite/LDH composite is an excellent adsorbent for the removal of MB from polluted water.