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To address the problem that traditional cement-based slurry materials cannot meet the actual demand for grouting and reinforcement of large deformation roadways in coal mines, some high-performance composite slurry materials are obtained by modifying ordinary Portland cement with nano-silica sol, ethylene-vinyl acetate copolymer (EVA) and fly ash. The orthogonal test and extreme difference analysis are used to systematically study the variation of the physical and mechanical properties of the composite slurries, determine the optimal ratio, and further analyze the difference in the physical properties between the optimal ratio of composite slurries and pure cement, construct the hydration reaction mechanism model of the composite slurries, and elucidate the mechanical properties of the composite slurries for reinforcing broken rocks. The results of the study show that the optimum proportion of composite slurry is 0.7 water-cement ratio, 15% fly ash, 2% silica sol and 7.5% EVA. Compared with pure cement, the rheology of composite slurry is slightly decreased, but the stability and mechanical properties of the slurry are significantly improved, with the initial setting time shortened by 38.9%, the final setting time shortened by 53.8%, the precipitation rate reduced by 60%, the stone rate increased by 3.3%, the uniaxial compressive strength increased by 39.1%, the tensile strength increased by 97.2%, and the tensile/compression ratio increased by 41.7%. Silica sol and fly ash undergo volcanic ash reaction with Ca(OH)2 to generate more calcium silicate hydrate (C-S-H) and calcium aluminate hydrate (C-A-H) at different times, which promotes the hydration reaction of the composite slurry and accelerates the film formation of EVA to make the stone body more dense. The injection volume of the composite grout and the uniaxial compressive strength of the bonded body both increase with the increasing grouting pressure. With the increase in the Talbot index, the compressive strength first increases and then decreases. The failure mode is often characterized by bulging, and shear dilation deformation is pronounced. When the grouting pressure exceeds 2 MPa and the Talbot index is 0.5, the bond strength of the grout is higher, and the damage is reduced. This study provides a feasible way for early strength and toughening modification of ce-mentitious composite pastes.