With a rapid increase in industrial growth around the world, the demand for an entirely novel category of nanoparticles and technologies for wastewater treatment has become a key concern for environmental protection. Recently, hybrids of layered double hydroxides (LDH), particularly those containing LDH, have gained attention as potential nanoscale adsorbents for water treatment. Recent research has shown that LDH-containing composites are interesting versatile materials with the ability to be used in energy storage, photocatalysis, nanocomposites, and water treatment. In the current work, LDH-containing composites were utilized as adsorbents for the purpose of purifying water. The adsorbents investigated are Zn–Co–Fe/LDH/Chitosan-in situ sample preparation (LDH/CS1) and Zn–Co–Fe/LDH/Chitosan-ex situ sample preparation (LDH/CS2). Furthermore, LDH/CS1 and LDH/CS2 were investigated for wastewater treatment from methyl orange dye (MO) with various adsorption conditions. When the initial MO concentration was 20 mg/L and the amount of adsorbent was 0.1 g, the removal efficiency reached 72.8 and 91.7% for LDH/CS1 and LDH/CS2, respectively. The MO’s maximum adsorption capabilities are 160.78 and 165.89 mg/g for LDH/CS1 and LDH/CS2, respectively, which is much greater than that of comparable commercial adsorbents. MO adsorption onto LDH/CS1 and LDH/CS2 was best characterized by the pseudo-second-order kinetic model. The equilibrium adsorption data was followed by the Freundlich and Langmuir models. The adsorption is favorable as evidenced by the equilibrium parameter RL values for MO adsorption onto LDH/CS1 and LDH/CS2, which were 0.227 and 0.144, respectively. Using the free volume distribution method and the positron annihilation lifetime technique, the nanostructure of the materials was examined.