The short-range hydrophobic interaction serves as a critical driving force in numerous interfacial physicochemical and biological processes, such as bubble-particle attachment, protein folding, and molecular self-assembly. However, a unified theoretical framework concerning its physical origin remains elusive, primarily due to the incomplete understanding of interfacial water behavior at the molecular level. In this study, we combined atomic force microscopy (AFM) with large-scale steered molecular dynamics (SMD) simulations to investigate the mechanism of the short-range hydrophobic force in an octadecyltrichlorosilane (OTS) self-assembled monolayer system with a water contact angle of approximately 100°. AFM force measurements reveal that the observable onset distance of the hydrophobic attraction is approximately 20 nm. Based on the EDLVO theory and a stepwise nonlinear least-squares fitting strategy, our analysis shows that the force magnitude decays exponentially with separation distance. The decay length is determined to be 1-2 nm, a characteristic that remains independent of the number of probe approach cycles. Furthermore, comparative experiments between air-saturated and partially degassed water demonstrate that variations in dissolved gas content do not alter the intrinsic parameters of the short-range hydrophobic force; additionally, experiments indicate that low concentrations of inorganic salt ions have no significant effect. Large-scale SMD simulations further demonstrate that when the hydrophobic particle approaches the substrate to a critical distance, the steering force manifests as a net attraction. Simultaneously, the confined region undergoes significant water molecule rearrangement and hydrogen bond network restructuring, accompanied by a precipitous drop in water density. This phenomenon is attributed to the inability of hydrophobic surfaces to form hydrogen bonds with adjacent water molecules, which induces the formation of a high-density, ordered hydrogen bond network. As the two surfaces approach, this structured network is disrupted, and the ordered water molecules are released into the bulk phase. This rearrangement of interfacial water molecules consequently gives rise to the short-range hydrophobic force. By integrating macroscopic AFM experiments with large-scale SMD simulations, this work reveals the mechanism of the short-range hydrophobic force based on solid-liquid interfacial water rearrangement, providing a solid theoretical foundation for understanding and modulating hydrophobic interactions at the molecular level.