Ensuring clean water sources is pivotal for sustainable development and the well-being of communities worldwide. This study represents a pioneering effort in water purification, exploring an innovative approach utilizing modified reduced graphene oxide (rGO) aerogels. These advanced materials promise to revolutionize environmental remediation efforts, specifically removing organic contaminants from aqueous solutions. The study investigates the exceptional adsorption properties of rGO-aerogel, enhanced with cysteamine, to understand its efficacy in addressing water pollution challenges. The characterization methods utilized encompass various analytical techniques, including FE-SEM, BET, FTIR, TGA, DSC, XPS, NMR, and elemental analysis. These analyses provide valuable insights into the material’s structural modifications and surface chemistry. The research comprehensively explores the intricacies of adsorption kinetics, equilibrium, and isothermal study to unravel the underlying mechanisms governing contaminant removal. MO and Ni2+ exhibited adsorption of 542.6 and 150.6 mg g−1, respectively, at 25 °C. Ni2+ has unveiled the highest removal at pH 5, and MO has shown high removal in a wide pH range (pH 4–7). Both contaminants have shown fast adsorption kinetic performance on an rGO-aerogel surface. This study aims to identify the synergistic effect of cysteamine and rGO in aerogel formation to remove heavy metals and organic contaminants. These findings mark a significant stride in advancing sustainable water-treatment methods and pioneering in synthesizing innovative materials with versatile applications in environmental contexts, offering a potential solution to the global water pollution crisis.