Abstract: To develop a novel high-strength and high-toughness inorganic anchoring material suitable for the support of surrounding rock in current roadway engineering, a composite anchoring system was prepared using superfine Portland cement as the binder, combined with calcium oxide expansive agent, sodium aluminate accelerator, and polycarboxylate superplasticizer. The system was toughened by the addition of alkali-resistant glass fiber (ARGF). A three-factor, three-level orthogonal experimental design was conducted using ARGF, expansive agent, and accelerator contents as variables, to evaluate the fluidity, setting time, volumetric expansion, and mechanical properties of the ARGF-enhanced superfine cement-based composite anchoring material (GFAP). XRD, FTIR, and SEM techniques were employed to analyze the hydration products, surface functional groups, and microstructural characteristics. Results showed that under a fixed water-cement ratio of 0.4 and 0.25% superplasticizer content, the optimal performance was achieved at 1% ARGF, 6% calcium oxide, and 4% sodium aluminate, yielding a fluidity of 221 mm, initial and final setting times of 182 min and 385 min, respectively, and a 3-day expansion rate of 0.5%, indicating micro-expansive behavior. The compressive strengths at 3 and 14 days were 58.3 MPa and 72.9 MPa, respectively, and the 14-day flexural strength reached 13.41 MPa, meeting the requirements for high early strength applications. Microscopic characterization confirmed that the mix proportions of additives significantly influenced the morphology, porosity, and compactness of hydration products. Under optimal conditions, ARGF formed a fiber-gel interlocking structure within the matrix, acted as a bridging agent, and promoted oriented C−S−H growth on its surface, enhancing interfacial bonding. The enhancement mechanism is attributed to the synergistic coupling among multi-component chemical additives, ARGF, and superfine cement. In full-length anchorage pull-out tests, the optimized GFAP system exhibited a high peak pull-out load(41.24 kN) and corresponding slip displacement(10.3 mm), with prolonged failure time, demonstrating strong resistance to failure and load-bearing capacity. In the tensile bonding strength test of coal body, the tensile bonding strength of the GFAP and coal bonding specimen with this ratio reached 0.66 MPa, demonstrating excellent interfacial bonding strength.