Water-soluble dyes are a common problem in wastewater treatment, requiring highly efficient methods for removal. In this study, novel sustainable adsorbents made from graphene-oxide (GO) and other materials, such as eggshell-derived calcium oxide nanoparticles (CaONPs-ES), fish bone calcium oxide nanoparticles (CaONPs-FB), and durian shell activated carbon (DSAC) were synthesized, characterized, and demonstrated for soluble dye removal from wastewater. Fermented maize grain extract (MES) was used as a green cross-linker in the synthesis process. The resulting nanocomposites, GO@CaONPs-ES/DSAC and GO@CaONPs-FB/DSAC, showed promising adsorption capabilities for methylene blue (MB) dye removal from aqueous environments. The prepared nanocomposites (GO@CaONPs-ES/DSAC and GO@CaONPs-FB/DSAC) were characterize using state-of-art instrumental techniques. The BET measurement revealed that the nanocomposites surface areas were enhanced due to the cross-linking phenomenon, improving their adsorption capability towards MB dye treatment. The adsorption data of GO@CaONPs-FB/DSAC and GO@CaONPs-ES/DSAC was well fitted to the Harkins-Jura and Freundlich models, respectively. The maximum sorption capacities of GO@CaONPs-ES/DSAC and GO@CaONPs-FB/DSAC were 1274.5 and 689.7 mg/g, respectively. The MB dye removal mechanism was driven by π-π interaction, hydrogen bonding, electrostatic attraction and physical interactions and the adsorption process of the nanocomposites followed pseudo-second-order kinetics. The adsorptive performance of the nanocomposites was stable, showing ∼96.45 % and ∼85.18 % after 10 successive cycles for GO@CaONPs-ES/DSAC and GO@CaONPs-FB/DSAC respectively. Cost evaluation revealed that bulk synthesis of GO@CaONPs-ES/DSAC and GO@CaONPs-FB/DSAC nanocomposites is cost-effective for treating large quantities of MB contaminated water and other potential dyes as well. Finally, the independent and synergetic contributions between pH, adsorbent dosage and temperature on MB removal by GO@CaONPs-ES/DSAC and GO@CaONPs-FB/DSAC were studied and optimized by central composite design (CCD) an aspect of the response surface methodology (RSM). Finally, this study suggests that the novel green cross-linking approach has a significant impact in enhancing the adsorptive performances of the developed nanocomposites to effectively capture MB from aqueous environment.