The irregular-shaped bone defect regeneration faces enormous challenges, which the bone tissue regeneration scaffolds with simultaneously angiogenesis and osteogenic mineralization displayed the great promise for bone defect repair. In this work, the functional peptides CP (FVDVT) with recruiting Ca2+ was prepared into the PLA/G@CP short fiber by electrospinning and homogenization, while the functional peptides BP (DRVQRQTTTVVA) with recruiting endogenous VEGF, which PLA/G and BP were both placed into the gelatin methacrylate (GM) solution to gain the GM@BCP hydrogels. Simultaneously, the BP could recruit endogenous vascular endothelial growth factor (VEGF), improve cell viability and cell proliferation, and as well as downregulate of the inflammatory environment to angiogenesis in whole transcriptome RNA sequencing of human umbilical vein endothelial cells (HUVECs), while PLA/G@CP short fiber could increase the mechanical behavior and promote bone matrix mineralization. The GM@BCP hydrogels showed the fit tissue-materials interface, biocompatible, non-toxic, and bioresorbable in vitro and in vivo. Thus, the calvarial defect model in SD rat showed the GM@BCP hydrogels passed great potential in promoting bone defect healing by inducing angiogenesis and mineralization at 8 weeks, which provides a novel platform for the bone defect regenerative repair.