To address the challenges of small diffusion radius, low early strength and long setting time of traditional cement grout in dense fine sand layer, based on the synergistic mechanism, a novel high-performance grouting material (HPGM) was developed using ground granulated blast-furnace slag (GGBS), ultra-fine fly ash (UFFA), and ultra-fine Portland cement (UFPC) as raw materials. Firstly, Laboratory experiments were conducted to investigate the working performance of HPGM under varying proportions. Secondly, based on the self-designed advanced small pipe grouting full-scale test device, the diffusion performance and reinforcement characteristics of HPGM under varying proportions were analyzed. Finally, the XRD and SEM testing methods were employed to elucidated the hydration mechanism of the HPGM. The test results indicate that as the mass ratio of GGBS to UFFA decreases, there is a gradual increase in hardening rate, fluidity and setting time of HPGM. Additionally, the unconfined compressive strength (UCS) initially increase before decreasing. Furthermore, with the decreased mass ratio of GGBS to UFFA, the HPGM diffused in dense fine sand layer through compaction-splitting, permeation-splitting, and splitting grouting processes. The hydration products of the HPGM primarily consist of C(-A)-S-H, AFt, and Ca(OH)2, when the mass ratio of GGBS to UFFA falls within the range of 4:2–3:3, the UFFA facilitates the AFt hydration products in significant quantities. Its cementation and filling effect lead to the formation of a dense microstructure in the soil, resulting in a substantial reduction in permeability coefficient and a marked increase in UCS. The research findings can offer high-performance grouting material for underground engineering construction while also presenting innovative ideas for resource utilization from solid wastes like GGBS and UFFA.