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To enhance the early-age properties of steel slag cement mortar and promote the resource utilization of metallurgical solid waste, in this study, nano-SiO2 (KH-NS) was modified using a KH550 silane coupling agent. The hydration kinetics and microstructure evolution were systematically analyzed by means of a macroscopic performance test (setting time and compressive strength) and multi-scale microscopic characterization (characterized by Fourier Transform Infrared Spectroscopy, Scanning Electron Microscopy, X-ray Diffraction, Thermogravimetry-Differential Thermal Analysis, and isothermal calorimetry). The influence mechanism of its content on the early performance of the steel slag cement system was systematically studied. Research findings indicate that at a given dosage, increasing the proportion of KH-NS results in a shorter setting time for steel slag mortar. When the KH-NS dosage reaches 1.5%, the initial and final setting times of steel slag mortar decrease by 24.21% and 21.20%, respectively. The addition of KH-NS effectively enhances the compressive strength of mortar, with a particularly pronounced effect on early strength prior to 14 h of curing. At a KH-NS dosage of 1.5%, the onset of the accelerated phase of hydration heat release in steel slag cement mortar is advanced by 2.5 h. Mechanistic studies indicate that KH-NS accelerates cement hydration by promoting C3S dissolution and C-S-H gel nucleation through interactions between surface silanol groups (Si-OH) and amino groups (-NH2). Furthermore, KH-NS refines the pore structure via a micro-aggregate filling effect, reducing the number of harmful pores and improving the pore size distribution. KH-NS continuously consumes Ca(OH)2 through pozzolanic reactions to generate C-S-H, with its reactivity increasing with higher dosage. Research confirms that KH-NS significantly enhances the early strength and density of steel slag mortar, providing both theoretical justification and technical support for developing low-carbon building materials based on solid waste with high dosage.