This study aims to investigate whether the combined use of thin sheet glass (FSG) and polyurethane acrylate (PUA) can enhance the mechanical properties and biocompatibility of glass ionomer cements (GICs) to improve the overall performance of commercial GICs. In this study, an innovative approach was employed by incorporating diluents and photoinitiators into PUA to develop a novel light-curable PUA material. The PUA was then used to modify the GIC to obtain PUA-modified GIC. Subsequently, physical and chemical methods were employed to corrode and chemically modify the glass fiber surface to acquire dried thin sheet glass (FSG). Different proportions of FSG (10%, 20%, and 30% by mass) were mixed with PUA-GIC to obtain FSG-PUA modified GIC. Mechanical and biocompatibility tests were conducted on regular GIC, PUA-GIC, resin-modified glass ionomer cement (RMGIC), and various proportions of FSG-PUA-GIC materials, including flexural strength, surface hardness, water absorption rate, solubility, shear strength, compressive strength (CS), in vitro cytotoxicity, as well as short-term oral toxicity and subcutaneous implantation trials. A novel FSG-PUA modified GIC was successfully prepared, which not only retained the excellent biocompatibility and fluoride ion release capacity of the original GIC but also significantly enhanced its mechanical strength and durability. The application of this innovative method provides a new direction for the development of dental restorative materials, particularly in addressing the shortcomings of GICs in terms of mechanical performance. The addition of FSG notably increased the flexural strength and surface hardness of GICs, especially at a 20% additive level, demonstrating superior performance compared with standard Fuji IX (F9) and slightly better than RMGIC. Water absorption rate and solubility initially decreased and then increased with an increase in FSG content, and significantly outperformed F9 and RMGIC at 10% and 20% additive levels. Shear strength and CS decreased with an increase in FSG content but remained superior to commercial groups. Material incubation with cells in vitro for 24-48 h showed no significant impact on cell viability, with cell viability exceeding 90%. Short-term oral toxicity tests demonstrated good biocompatibility of the material, and subcutaneous implant trials did not observe any significant inflammation or pathological changes within 12 weeks of observation. The use of FSG-PUA materials effectively enhances the mechanical properties of GIC materials, demonstrating excellent biocompatibility and significant potential as dental restorative materials. Among them, the 20% FSG-PUA modified GICs exhibited significantly superior flexural strength, surface hardness, shear strength, water absorption, and solubility compared with F9 and slightly surpassing RMGIC, showcasing the best mechanical performance.