In this work, three solid adsorbents were synthesized, namely, nanozeolite-Y prepared from rice husks ash by a sol-gel method as a green biosource (ZN), chitosan as a cationic biopolymer (CS), and nanozeolite-Y/chitosan composite (CSZ). An eco-friendly composite that consists of chitosan and nanozeolite-Y was used to combine the advantages of nanoparticles with biopolymers two materials to increase the removal % of methylene blue dye. All the synthetized solid adsorbents were investigated using TGA, nitrogen adsorption, SEM, TEM, FTIR, XRD, and zeta potential. The results showed that CSZ particles had a high specific surface area (432.3 m2/g), mesoporosity (with an average pore diameter of 2.59 nm), a smaller TEM particle size (between 28.6 and 60.7 nm), a lot of chemical functional groups, and high thermal stability. CSZ exhibited the maximum adsorption capacity (141.04 mg/g) towards methylene blue. The adsorption nature of methylene blue onto CS and CSZ is endothermic, spontaneous, and a physical adsorption process, while it is exothermic, nonspontaneous, physical adsorption process in the case of ZN, as confirmed by thermodynamic results. Pseudo-second order, Elovich, Dubinin-Radushkevich, Freundlich, Langmuir, Temkin, and adsorption models all fit the MB adsorption well, with correlation coefficients reaching about 0.9997. Nitric acid was found to be the best desorbing agent, with a desorption efficiency of about 99%.