Carbon-based nanostructures are promising eco-friendly multifunctional nanomaterials because of their tunable surface and optoelectronic properties for a variety of energy and environmental applications. The present study focuses on the synthesis of graphene oxide (GO) with particular emphasis on engineering its surface and optical properties for making it an excellent adsorbent as well as a visible light-active photocatalyst. It was achieved by modifying the improved Hummers method through optimizing the synthesis parameters involved in the oxidation process. This controlled synthesis allows for systematic tailoring of structural, optical, and surface functionality, leading to improved adsorption and photocatalytic properties for the sustainable removal of organic pollutants in water treatment. Several spectroscopic and microscopic characterization techniques, such as XRD, SEM, Raman, UV-visible, FTIR, TEM, XPS, BET, etc. were employed to analyze the degree of oxidation, surface chemistry/functionalization, morphological, optical, and structural properties of the synthesized GO nanostructures. The analyses showed excellent surface functionality with surface active sites for better adsorptive removal and a tunable band gap from 2.51 to 2.76 eV exhibiting excellent natural sunlight activity (>99%) for photocatalytic removal of the organic pollutant. Various adsorption isotherms have been studied with excellent adsorption capability (Qmax = 454.54 mg/g) as compared to the literature. The study introduces GO both as a proficient stand-alone (sole) nanoadsorbent as well as a nanophotocatalyst for the efficient removal of organic dye pollutants in water treatment. Additionally, the article highlights the sustainable solar light-induced green chemistry aspects of GO as an excellent recyclable adsorbent as a result of its self-cleaning ability under natural sunlight, demonstrating its potential in real eco-friendly environmental and practical applications.