Graphene oxide quantum dots (GOQDs) possess excellent biocompatibility and have shown potential to enhance osteogenesis and angiogenesis. The objective of this work was to construct Ti6Al4V porous scaffolds modified with different GOQD concentrations and investigate their influence on osteogenesis and angiogenesis. Porous Ti6Al4V scaffolds were coated with GOQDs at concentrations of 0.1, 1, and 10 μg/mL. The proliferation and adhesion of bone marrow mesenchymal stem cells (BMSCs) and human umbilical vein endothelial cells (HUVECs) on these scaffolds were evaluated using CCK-8 assay, immunofluorescence staining, and RT-PCR. In vivo bone regeneration and angiogenesis were assessed through micro-CT imaging, Tissue section staining analysis. The results showed successful deposition of GOQDs and the presence of characteristic functional groups. In vitro assays results demonstrated that scaffolds coated with 0.1 μg/mL GOQDs significantly promoted the osteogenic/angiogenic differentiation of BMSCs and HUVECs. In vivo experiments results revealed that the 0.1 μg/mL GOQDs-coated scaffold (GQ@TC4) significantly enhanced bone formation and vascularization after 12 weeks. These findings suggest that Ti6Al4V biomimetic porous scaffolds functionalized with an optimal concentration (0.1 μg/mL) of GOQDs can effectively promote both osteogenesis and angiogenesis, offering a promising strategy for bone defect repair.