An improvement to Hummers' method involving a cascade-design graphite oxidation reaction is reported to optimize safety and efficiency in the production of graphite oxide (GrO) and graphene oxide (GO). Chemical reduction using highly alkaline ammonia solution is a novel approach to synthesizing reduced graphene oxide (RGO). In this original research, we revisit the oxidation and reduction reactions, providing significant findings regarding the synthetic pathway to obtain a bioinspired water-intercalated hydrogel of RGO nanosheets. Influential factors in the graphite oxidation reaction, typically the exothermic reaction temperature and hydrogen peroxide effect, are described. Furthermore, the chemical reaction of GO reduction using highly alkaline ammonia solution (pH 14) was investigated to produce hydrated RGO nanosheets assembled in a hydrogel structure (97% water). Three-dimensional assembly and water intercalation are key to preserve the non-stacking state of RGO nanosheets. Therefore, ultrasound transmission to aqueous channels in the macroscopic RGO hydrogel vibrated and dispersed the RGO nanosheets in water. Analytical results revealed the single-layer nanostructures, functional groups, optical band gaps, optimized C/O ratios, particle sizes and zeta potentials of GO and RGO nanosheets. The reversible self-assembly of RGO hydrogels is essential for many applications, such as RGO coatings and polymer/RGO nanocomposites. In a water purification application, the RGO hydrogel was dispersed in aqueous solution by simple agitation and showed a high capacity for organic dye adsorption. After the adsorption, the RGO/dye particles were easily removed by filtration through ordinary cellulose paper. The process of adsorption and filtration is effective and inexpensive for practical environmental remediation. In summary, a bioinspired structure of RGO hydrogel is conceptualized for prospective nanotechnology.