The removal of organic dye effluents released from numerous dye-utilizing industries is of increasing concern. In this study, the efficiency of wastewater dye adsorption methods was studied by synthesizing and characterizing MoS2-COOH @ UiO-66-NH2 composite based on a novel type of transition metal dichalcogenide/metal-organic frameworks (TMD/MOF) prepared using basic materials such as MoS2, and UiO-66-NH2. The fabricated MoS2-COOH @ UiO-66-NH2 composite was characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), thermal stability (TGA), FT-IR spectroscopy, and Energy Dispersive X-ray mapping analysis. In addition, the surface charge of the nanocomposite was probed with Zeta potential (ζ) measurements using the Dynamic Light Scattering (DLS) technique. TMD/MOF composites, as adsorbents, were investigated under various experimental conditions and their equilibrium adsorption capacity towards MB was found to be up to 253mgg−1 (when pH = 7.0, contact time was 100 min, the adsorbent dose was 6 mg and initial MB concentration was 75 mgL − 1 (30 ml) Using the pseudo-first-order and pseudo-second-order models to study the kinetic behavior of the adsorption process, a better performance of the pseudo-second-order model in describing the kinetic behavior of the MB and MO adsorption process was observed. In addition, MoS2-COOH @ UiO-66-NH2 composites could selectively separate methylene blue from a mixture of MB (methylene blue) and MO (methyl orange) with a separation efficiency of 86%.