Nanomaterials play as ignificant role in adsorption treatment of dye wastewater,b ut irreversible aggregation of nanoparticles poses as ignificant problem. In this work, nanomesoporous zinc-doped silicate (NMSZ) was prepared by an in situ method. To preventa gglomeration, NMSZ was covalently bonded to grapheneo xide (GO) sheets to form a nano-silica/zinc/grapheneo xide composite (GO-NMSZ), aimed at removal of cationic dye methylene blue (MB). For comparison, undoped mesoporouss ilica (MS) was also synthesizeda nd modifiedt oo btain as ilica/graphene oxide composite (GO-MS). The materials were characterized by powderX RD, SEM, FTIR spectroscopy,T EM, nitrogen sorp-tion, and X-ray photoelectron spectroscopy (XPS). Preservation of the oxygen-containingg roups of GO in the composites led to highera dsorptioncapacities. The best GO-NMSZ composite exhibited an enhanced adsorption capacity of 100.4 mg g Ă1 for MB compared to those of undoped GO-MS (80.1 mg g Ă1 )a nd nongrafted NMSZ (55.7 mg g Ă1 ). The nonselectivec haracter of GO-NMSZ is demonstrated by effective adsorption of anionic dye Congo red (127.4 mg g Ă1 )a nd neutral dyei satin (289.0 mg g Ă1 ). The adsorption kinetics, adsorptioni sotherms,a nd at hermodynamic study suggested that MB adsorption occurs by chemisorptiona nd is endothermic in nature.