The present study focuses on the synthesis of several graphene oxide nanosheet (GON)-based dispersants with an adsorption mode of “surface-to-surface” for the preparation of Shenhua coal (SC) water slurry (SCWS), achieved by grafting allyl polyoxyethylene ether (APEG) onto GON edges with varying degrees of oxidation using emulsion polymerization and esterification techniques. The impacts of the oxidation degree of GON on its structural characteristics and the performance of GON-based dispersants in SCWS were comprehensively assessed through a range of experimental techniques, alongside molecular dynamics (MD) simulations. Results demonstrated that with the increase in oxidation degree, there was an elevation of oxygen-containing groups, in which the content of COH decreased while the content of COC increased. Among all dispersants, GA-2, which was synthesized using GON-2 as the raw material with a graphite-to-KMnO4 mass ratio of 1:2.5, exhibited superior viscosity-reducing and stabilizing abilities compared to other dispersants. All SCWSs demonstrated pseudoplastic fluid behavior and showed good agreement with the Herschel-Bulkley model. After the adsorption of dispersants in SC, both the Zeta potential and surface wettability of SC significantly improved, especially with GA-2. The interaction mechanism between the dispersant and SC was analyzed by establishing and employing three adsorption models (M-1, M-2, and M-3). The interfacial adsorption structure confirmed that the dispersant exhibited “surface-to-surface” mode on coal through hydrophobic interaction, hydrogen bonding, and π–π interaction. Energy studies revealed that M-2 with the highest Eads (−105.31 kcal/mol) demonstrated superior adsorption strength compared to M-1 and M-3. Investigations into water molecule mobility revealed that the interaction between the GON-based dispersant and SC resulted in a reduction of water molecule mobility, thereby promoting water molecule aggregation to facilitate the formation of hydration films and enhance SCWS stability. In summary, an optimal oxidation degree of GON was found to be crucial for enhancing the performance of GON-based dispersants; higher oxidation levels may hinder dispersant adsorption on coal surfaces by converting hydroxyl and carboxyl groups into epoxide groups, thus impairing the conjugated structure.